In his decade in charge of the National, Olivier acted in thirteen plays and directed eight. Several of the roles he played were minor characters, including a crazed butler in Feydeau's A Flea in Her Ear and a pompous solicitor in Maugham's Home and Beauty; the vulgar soldier Captain Brazen in Farquhar's 1706 comedy The Recruiting Officer was a larger role but not the leading one. Apart from his Astrov in the Uncle Vanya, familiar from Chichester, his first leading role for the National was Othello, directed by Dexter in 1964. The production was a box-office success and was revived regularly over the next five seasons. His performance divided opinion. Most of the reviewers and theatrical colleagues praised it highly; Franco Zeffirelli called it "an anthology of everything that has been discovered about acting in the past three centuries." Dissenting voices included The Sunday Telegraph, which called it "the kind of bad acting of which only a great actor is capable ... near the frontiers of self-parody"; the Director Jonathan Miller thought it "a condescending view of an Afro Caribbean person". The burden of playing this demanding part at the same time as managing the new company and planning for the move to the new theatre took its toll on Olivier. To add to his load, he felt obliged to take over as Solness in The Master Builder when the ailing Redgrave withdrew from the role in November 1964. For the first time Olivier began to suffer from stage fright, which plagued him for several years. The National Theatre production of Othello was released as a film in 1965, which earned four Academy Award nominations, including another for Best Actor for Olivier.

Olivier was born in Dorking, Surrey, the youngest of the three children of the Revd Gerard Kerr Olivier (1869–1939) and his wife Agnes Louise, née Crookenden (1871–1920). Their elder children were Sybille (1901–1989) and Gerard Dacres "Dickie" (1904–1958). His great-great-grandfather was of French Huguenot descent, and Olivier came from a long line of Protestant clergymen. Gerard Olivier had begun a career as a schoolmaster, but in his thirties he discovered a strong religious vocation and was ordained as a priest of the Church of England. He practised extremely high church, ritualist Anglicanism and liked to be addressed as "Father Olivier". This made him unacceptable to most Anglican congregations, and the only church posts he was offered were temporary, usually deputising for regular incumbents in their absence. This meant a nomadic existence, and for Laurence's first few years, he never lived in one place long enough to make friends.

In 1912, when Olivier was five, his Father secured a permanent appointment as assistant priest at St Saviour's, Pimlico. He held the post for six years, and a stable family life was at last possible. Olivier was devoted to his mother, but not to his Father, whom he found a cold and remote parent. Nevertheless, he learned a great deal of the art of performing from him. As a young man Gerard Olivier had considered a stage career and was a dramatic and effective preacher. Olivier wrote that his Father knew "when to drop the voice, when to bellow about the perils of hellfire, when to slip in a gag, when suddenly to wax sentimental ... The quick changes of mood and manner absorbed me, and I have never forgotten them."

In 1916, after attending a series of preparatory schools, Olivier passed the singing examination for admission to the choir school of All Saints, Margaret Street, in central London. His elder brother was already a pupil, and Olivier gradually settled in, though he felt himself to be something of an outsider. The church's style of worship was (and remains) Anglo-Catholic, with emphasis on ritual, vestments and incense. The theatricality of the services appealed to Olivier, and the vicar encouraged the students to develop a taste for secular as well as religious drama. In a school production of Julius Caesar in 1917, the ten-year-old Olivier's performance as Brutus impressed an audience that included Lady Tree, the young Sybil Thorndike, and Ellen Terry, who wrote in her diary, "The small boy who played Brutus is already a great actor." He later won praise in other schoolboy productions, as Maria in Twelfth Night (1918) and Katherine in The Taming of the Shrew (1922).

From All Saints, Olivier went on to St Edward's School, Oxford, from 1920 to 1924. He made little mark until his final year, when he played Puck in the school's production of A Midsummer Night's Dream; his performance was a tour de force that won him popularity among his fellow pupils. In January 1924, his brother left England to work in India as a rubber planter. Olivier missed him greatly and asked his Father how soon he could follow. He recalled in his memoirs that his Father replied, "Don't be such a fool, you're not going to India, you're going on the stage."

In 1924 Gerard Olivier, a habitually frugal man, told his son that not only must he gain admission to the Central School of Speech Training and Dramatic Art, but he must also gain a scholarship with a bursary to cover his tuition fees and living expenses. Olivier's sister had been a student there and was a favourite of Elsie Fogerty, the founder and principal of the school. Olivier later speculated that it was on the strength of this that Fogerty agreed to award him the bursary.

One of Olivier's contemporaries at the school was Peggy Ashcroft, who observed he was "rather uncouth in that his sleeves were too short and his hair stood on end but he was intensely lively and great fun". By his own admission, he was not a very conscientious student, but Fogerty liked him and later said that he and Ashcroft stood out among her many pupils. On leaving the school after a year, Olivier gained work with small touring companies before being taken on in 1925 by Sybil Thorndike and her husband, Lewis Casson, as a bit-part player, understudy and assistant stage manager for their London company. He modelled his performing style on that of Gerald du Maurier, of whom he said, "He seemed to mutter on stage but had such perfect technique. When I started I was so busy doing a du Maurier that no one ever heard a word I said. The Shakespearean actors one saw were terrible hams like Frank Benson." His concern to speak naturally and avoid what he called "singing" Shakespeare's verse was the cause of much frustration in his early career, with critics regularly decrying his delivery.

In 1926, on Thorndike's recommendation, Olivier joined the Birmingham Repertory Company. His biographer Michael Billington describes the Birmingham company as "Olivier's university", where in his second year he was given the chance to play a wide range of important roles, including Tony Lumpkin in She Stoops to Conquer, the title role in Uncle Vanya, and Parolles in All's Well That Ends Well. Billington adds that the engagement led to "a lifelong friendship with his fellow actor Ralph Richardson that was to have a decisive effect on the British theatre."

In 1928 Olivier created the role of Stanhope in R. C. Sherriff's Journey's End, in which he scored a great success at its single Sunday night premiere. He was offered the part in the West End production the following year, but turned it down in favour of the more glamorous role of Beau Geste in a stage adaptation of P. C. Wren's 1929 novel of the same name. Journey's End became a long-running success; Beau Geste failed. The Manchester Guardian commented, "Mr. Laurence Olivier did his best as Beau, but he deserves and will get better parts. Mr. Olivier is going to make a big name for himself". For the rest of 1929 Olivier appeared in seven plays, all of which were short-lived. Billington ascribes this failure rate to poor choices by Olivier rather than mere bad luck.

In 1930 Noël Coward cast Olivier as Victor Prynne in his new play Private Lives, which opened at the new Phoenix Theatre in London in September. Coward and Gertrude Lawrence played the lead roles, Elyot Chase and Amanda Prynne. Victor is a secondary character, along with Sybil Chase; the author called them "extra puppets, lightly wooden ninepins, only to be repeatedly knocked down and stood up again". To make them credible spouses for Amanda and Elyot, Coward was determined that two outstandingly attractive performers should play the parts. Olivier played Victor in the West End and then on Broadway; Adrianne Allen was Sybil in London, but could not go to New York, where the part was taken by Esmond. In addition to giving the 23-year-old Olivier his first successful West End role, Coward became something of a mentor. In the late 1960s Olivier told Sheridan Morley:

In 1931 RKO Pictures offered Olivier a two-film contract at $1,000 a week; he discussed the possibility with Coward, who, irked, told Olivier "You've no artistic integrity, that's your trouble; this is how you cheapen yourself." He accepted and moved to Hollywood, despite some misgivings. His first film was the drama Friends and Lovers, in a supporting role, before RKO loaned him to Fox Studios for his first film lead, a British Journalist in a Russia under martial law in The Yellow Passport, alongside Elissa Landi and Lionel Barrymore. The cultural Historian Jeffrey Richards describes Olivier's look as an attempt by Fox Studios to produce a likeness of Ronald Colman, and Colman's moustache, voice and manner are "perfectly reproduced". Olivier returned to RKO to complete his contract with the 1932 drama Westward Passage, which was a commercial failure. Olivier's initial foray into American films had not provided the breakthrough he hoped for; disillusioned with Hollywood, he returned to London, where he appeared in two British films, Perfect Understanding with Gloria Swanson and No Funny Business—in which Esmond also appeared. He was tempted back to Hollywood in 1933 to appear opposite Greta Garbo in Queen Christina, but was replaced after two weeks of filming because of a lack of chemistry between the two.

Olivier's stage roles in 1934 included Bothwell in Gordon Daviot's Queen of Scots, which was only a moderate success for him and for the play, but led to an important engagement for the same management (Bronson Albery) shortly afterwards. In the interim he had a great success playing a thinly disguised version of the American actor John Barrymore in Edna Ferber's Theatre Royal. His success was vitiated by his breaking an ankle two months into the run, in one of the athletic, acrobatic Stunts with which he liked to enliven his performances.

In 1935, under Albery's management, John Gielgud staged Romeo and Juliet at the New Theatre, co-starring with Peggy Ashcroft, Edith Evans and Olivier. Gielgud had seen Olivier in Queen of Scots, spotted his potential, and now gave him a major step up in his career. For the first weeks of the run Gielgud played Mercutio and Olivier played Romeo, after which they exchanged roles. The production broke all box-office records for the play, running for 189 performances. Olivier was enraged at the notices after the first night, which praised the virility of his performance but fiercely criticised his speaking of Shakespeare's verse, contrasting it with his co-star's mastery of the poetry. The friendship between the two men was prickly, on Olivier's side, for the rest of his life.

Following Olivier's success in Shakespearean stage productions, he made his first foray into Shakespeare on film in 1936, as Orlando in As You Like It, directed by Paul Czinner, "a charming if lightweight production", according to Michael Brooke of the British Film Institute's (BFI's) Screenonline. The following year Olivier appeared alongside Vivien Leigh in the historical drama Fire Over England. He had first met Leigh briefly at the Savoy Grill and then again when she visited him during the run of Romeo and Juliet, probably early in 1936, and the two had begun an affair sometime that year. Of the relationship, Olivier later said that "I couldn't help myself with Vivien. No man could. I hated myself for cheating on Jill, but then I had cheated before, but this was something different. This wasn't just out of lust. This was love that I really didn't ask for but was drawn into." While his relationship with Leigh continued he conducted an affair with the Actress Ann Todd, and possibly had a brief affair with the actor Henry Ainley, according to the biographer Michael Munn.

In June 1937 the Old Vic company took up an invitation to perform Hamlet in the courtyard of the castle at Elsinore, where Shakespeare located the play. Olivier secured the casting of Leigh to replace Cherry Cottrell as Ophelia. Because of torrential rain the performance had to be moved from the castle courtyard to the ballroom of a local hotel, but the tradition of playing Hamlet at Elsinore was established, and Olivier was followed by, among others, Gielgud (1939), Redgrave (1950), Richard Burton (1954), Derek Jacobi (1979), Kenneth Branagh (1988) and Jude Law (2009). Back in London, the company staged Macbeth, with Olivier in the title role. The stylised production by Michel Saint-Denis was not well liked, but Olivier had some good notices among the bad. On returning from Denmark, Olivier and Leigh told their respective spouses about the affair and that their marriages were over; Esmond moved out of the marital house and in with her mother. After Olivier and Leigh made a tour of Europe in mid 1937 they returned to separate film projects—A Yank at Oxford for her and The Divorce of Lady X for him—and moved into a property together in Iver, Buckinghamshire.

In 1938 Olivier joined Richardson to film the spy thriller Q Planes, released the following year. Frank Nugent, the critic for The New York Times, thought Olivier was "not quite so good" as Richardson, but was "quite acceptable". In late 1938, lured by a salary of $50,000, the actor travelled to Hollywood to take the part of Heathcliff in the 1939 film Wuthering Heights, alongside Merle Oberon and David Niven. In less than a month Leigh had joined him, explaining that her trip was "partially because Larry's there and partially because I intend to get the part of Scarlett O'Hara"—the role in Gone with the Wind in which she was eventually cast. Olivier did not enjoy making Wuthering Heights, and his approach to film acting, combined with a dislike for Oberon, led to tensions on set. The Director, william Wyler, was a hard taskmaster, and Olivier learned to remove what Billington described as "the carapace of theatricality" to which he was prone, replacing it with "a palpable reality". The resulting film was a commercial and critical success that earned him a nomination for the Academy Award for Best Actor, and created his screen reputation. Caroline Lejeune, writing for The Observer, considered that "Olivier's dark, moody face, abrupt style, and a certain fine arrogance towards the world in his playing are just right" in the role, while the reviewer for The Times wrote that Olivier "is a good embodiment of Heathcliff ... impressive enough on a more human plane, speaking his lines with real distinction, and always both romantic and alive."

After returning to London briefly in mid-1939, the couple returned to America, Leigh to film the final takes for Gone with the Wind, and Olivier to prepare for filming of Alfred Hitchcock's Rebecca—although the couple had hoped to appear in it together. Instead, Joan Fontaine was selected for the role of Mrs de Winter, as the Producer David O. Selznick thought that not only was she more suitable for the role, but that it was best to keep Olivier and Leigh apart until their divorces came through. Olivier followed Rebecca with Pride and Prejudice, in the role of Mr. Darcy. To his disappointment Elizabeth Bennet was played by Greer Garson rather than Leigh. He received good reviews for both films and showed a more confident screen presence than he had in his early work. In January 1940 Olivier and Esmond were granted their divorce. In February, following another request from Leigh, her husband also applied for their marriage to be terminated.

On stage, Olivier and Leigh starred in Romeo and Juliet on Broadway. It was an extravagant production, but a commercial failure. In The New York Times Brooks Atkinson praised the scenery but not the acting: "Although Miss Leigh and Mr Olivier are handsome young people they hardly act their parts at all." The couple had invested almost all their savings in the project, and its failure was a grave financial blow. They were married in August 1940, at the San Ysidro Ranch in Santa Barbara.

Throughout the war Tyrone Guthrie had striven to keep the Old Vic company going, even after German bombing in 1942 left the theatre a near-ruin. A small troupe toured the provinces, with Sybil Thorndike at its head. By 1944, with the tide of the war turning, Guthrie felt it time to re-establish the company in a London base and invited Richardson to head it. Richardson made it a condition of accepting that he should share the acting and management in a triumvirate. Initially he proposed Gielgud and Olivier as his colleagues, but the former declined, saying, "It would be a disaster, you would have to spend your whole time as Referee between Larry and me." It was finally agreed that the third member would be the stage Director John Burrell. The Old Vic governors approached the Royal Navy to secure the release of Richardson and Olivier; the Sea Lords consented, with, as Olivier put it, "a speediness and lack of reluctance which was positively hurtful."

In 1943, at the behest of the Ministry of Information, Olivier began working on Henry V. Originally he had no intention of taking the directorial duties, but ended up directing and producing, in addition to taking the title role. He was assisted by an Italian internee, Filippo Del Giudice, who had been released to produce propaganda for the Allied cause. The decision was made to film the battle scenes in neutral Ireland, where it was easier to find the 650 extras. John Betjeman, the press attaché at the British embassy in Dublin, played a key liaison role with the Irish government in making suitable arrangements. The film was released in November 1944. Brooke, writing for the BFI, considers that it "came too late in the Second World War to be a call to arms as such, but formed a powerful reminder of what Britain was defending." The music for the film was written by william Walton, "a score that ranks with the best in film music", according to the music critic Michael Kennedy. Walton also provided the music for Olivier's next two Shakespearean adaptations, Hamlet (1948) and Richard III (1955). Henry V was warmly received by critics. The reviewer for The Manchester Guardian wrote that the film combined "new art hand-in-hand with old genius, and both superbly of one mind", in a film that worked "triumphantly". The critic for The Times considered that Olivier "plays Henry on a high, heroic note and never is there danger of a crack", in a film described as "a triumph of film craft". There were Oscar nominations for the film, including Best Picture and Best Actor, but it won none and Olivier was instead presented with a "Special Award". He was unimpressed, and later commented that "this was my first absolute fob-off, and I regarded it as such."

The second season, in 1945, featured two double bills. The first consisted of Henry IV, Parts 1 and 2. Olivier played the warrior Hotspur in the first and the doddering Justice Shallow in the second. He received good notices, but by general consent the production belonged to Richardson as Falstaff. In the second double bill it was Olivier who dominated, in the title roles of Oedipus Rex and The Critic. In the two one-act plays his switch from searing tragedy and horror in the first half to farcical comedy in the second impressed most critics and audience members, though a minority felt that the transformation from Sophocles's bloodily blinded hero to Sheridan's vain and ludicrous Mr Puff "smacked of a quick-change turn in a music hall". After the London season the company played both the double bills and Uncle Vanya in a six-week run on Broadway.

From academic and other institutions, Olivier received honorary doctorates from the university of Tufts, Massachusetts (1946), Oxford (1957) and Edinburgh (1964). He was also awarded the Danish Sonning Prize in 1966, the Gold Medallion of the Royal Swedish Academy of Letters, History and Antiquities in 1968; and the Albert Medal of the Royal Society of Arts in 1976.

For his work in films, Olivier received four Academy Awards: an honorary award for Henry V (1947), a Best Actor award and one as Producer for Hamlet (1948), and a second honorary award in 1979 to recognise his lifetime of contribution to the art of film. He was nominated for nine other acting Oscars and one each for production and direction. He also won two British Academy Film Awards out of ten nominations, five Emmy Awards out of nine nominations, and three Golden Globe Awards out of six nominations. He was nominated once for a Tony Award (for best actor, as Archie Rice) but did not win.

In 1948 Olivier led the Old Vic company on a six-month tour of Australia and New Zealand. He played Richard III, Sir Peter Teazle in Sheridan's The School for Scandal and Antrobus in Thornton Wilder's The Skin of Our Teeth, appearing alongside Leigh in the latter two plays. While Olivier was on the Australian tour and Richardson was in Hollywood, Esher terminated the contracts of the three Directors, who were said to have "resigned". Melvyn Bragg in a 1984 study of Olivier, and John Miller in the authorised biography of Richardson, both comment that Esher's action put back the establishment of a National Theatre for at least a decade. Looking back in 1971, Bernard Levin wrote that the Old Vic company of 1944 to 1948 "was probably the most illustrious that has ever been assembled in this country". The Times said that the triumvirate's years were the greatest in the Old Vic's history; as The Guardian put it, "the governors summarily sacked them in the interests of a more mediocre company spirit".

Although it was Common knowledge that the Old Vic triumvirate had been dismissed, they refused to be drawn on the matter in public, and Olivier even arranged to play a final London season with the company in 1949, as Richard III, Sir Peter Teazle, and Chorus in his own production of Anouilh's Antigone with Leigh in the title role. After that, he was free to embark on a new career as an actor-manager. In partnership with Binkie Beaumont he staged the English premiere of Tennessee Williams's A Streetcar Named Desire, with Leigh in the central role of Blanche DuBois. The play was condemned by most critics, but the production was a considerable commercial success, and led to Leigh's casting as Blanche in the 1951 film version. Gielgud, who was a devoted friend of Leigh's, doubted whether Olivier was wise to let her play the demanding role of the mentally unstable heroine: "[Blanche] was so very like her, in a way. It must have been a most dreadful strain to do it night after night. She would be shaking and white and quite distraught at the end of it."

The Oliviers' marriage was disintegrating during the late 1950s. While directing Charlton Heston in the 1960 play The Tumbler, Olivier divulged that "Vivien is several thousand miles away, trembling on the edge of a cliff, even when she's sitting quietly in her own drawing room", at a time when she was threatening suicide. In May 1960 divorce proceedings started; Leigh reported the fact to the press and informed reporters of Olivier's relationship with Plowright. The decree nisi was issued in December 1960, which enabled him to marry Plowright in March 1961. A son, Richard, was born in December 1961; two daughters followed, Tamsin Agnes Margaret—born in January 1963—and Julie-Kate, born in July 1966.

While Leigh made Streetcar in 1951, Olivier joined her in Hollywood to film Carrie, based on the controversial novel Sister Carrie; although the film was plagued by troubles, Olivier received warm reviews and a BAFTA nomination. Olivier began to notice a change in Leigh's behaviour, and he later recounted that "I would find Vivien sitting on the corner of the bed, wringing her hands and sobbing, in a state of grave distress; I would naturally try desperately to give her some comfort, but for some time she would be inconsolable." After a holiday with Coward in Jamaica, she seemed to have recovered, but Olivier later recorded, "I am sure that ... [the doctors] must have taken some pains to tell me what was wrong with my wife; that her disease was called manic depression and what that meant—a possibly permanent cyclical to-and-fro between the depths of depression and wild, uncontrollable mania. He also recounted the years of problems he had experienced because of Leigh's illness, writing, "throughout her possession by that uncannily evil Monster, manic depression, with its deadly ever-tightening spirals, she retained her own individual canniness—an ability to disguise her true mental condition from almost all except me, for whom she could hardly be expected to take the trouble."

For the Coronation season of 1953, Olivier and Leigh starred in the West End in Terence Rattigan's Ruritanian comedy, The Sleeping Prince. It ran for eight months but was widely regarded as a minor contribution to the season, in which other productions included Gielgud in Venice Preserv'd, Coward in The Apple Cart and Ashcroft and Redgrave in Antony and Cleopatra.

Olivier directed his third Shakespeare film in September 1954, Richard III (1955), which he co-produced with Korda. The presence of four theatrical knights in the one film—Olivier was joined by Cedric Hardwicke, Gielgud and Richardson—led an American reviewer to dub it "An-All-Sir-Cast". The critic for The Manchester Guardian described the film as a "bold and successful achievement", but it was not a box-office success, which accounted for Olivier's subsequent failure to raise the funds for a planned film of Macbeth. He won a BAFTA award for the role and was nominated for the Best Actor Academy Award, which Yul Brynner won.

In their third production of the 1955 Stratford season, Olivier played the title role in Titus Andronicus, with Leigh as Lavinia. Her notices in the part were damning, but the production by Peter Brook and Olivier's performance as Titus received the greatest ovation in Stratford history from the first-night audience, and the critics hailed the production as a landmark in post-war British theatre. Olivier and Brook revived the production for a continental tour in June 1957; its final performance, which closed the old Stoll Theatre in London, was the last time Leigh and Olivier acted together.

Leigh became pregnant in 1956 and withdrew from the production of Coward's comedy South Sea Bubble. The day after her final performance in the play she miscarried and entered a period of depression that lasted for months. The same year Olivier decided to direct and produce a film version of The Sleeping Prince, retitled The Prince and the Showgirl. Instead of appearing with Leigh, he cast Marilyn Monroe as the showgirl. Although the filming was challenging because of Monroe's behaviour, the film was appreciated by the critics.

Olivier received another BAFTA nomination for his supporting role in 1959's The Devil's Disciple. The same year, after a gap of two decades, Olivier returned to the role of Coriolanus, in a Stratford production directed by the 28-year-old Peter Hall. Olivier's performance received strong praise from the critics for its fierce athleticism combined with an emotional vulnerability. In 1960 he made his second appearance for the Royal Court company in Ionesco's absurdist play Rhinoceros. The production was chiefly remarkable for the star's quarrels with the Director, Orson Welles, who according to the biographer Francis Beckett suffered the "appalling treatment" that Olivier had inflicted on Gielgud at Stratford five years earlier. Olivier again ignored his Director and undermined his authority. In 1960 and 1961 Olivier appeared in Anouilh's Becket on Broadway, first in the title role, with Anthony Quinn as the king, and later exchanging roles with his co-star.

In February 1960, for his contribution to the film industry, Olivier was inducted into the Hollywood Walk of Fame, with a star at 6319 Hollywood Boulevard; he is included in the American Theater Hall of Fame. In 1977 Olivier was awarded a British Film Institute Fellowship.

In 1961 Olivier accepted the directorship of a new theatrical venture, the Chichester Festival. For the opening season in 1962 he directed two neglected 17th-century English plays, John Fletcher's 1638 comedy The Chances and John Ford's 1633 tragedy The Broken Heart, followed by Uncle Vanya. The company he recruited was forty strong and included Thorndike, Casson, Redgrave, Athene Seyler, John Neville and Plowright. The first two plays were politely received; the Chekhov production attracted rapturous notices. The Times commented, "It is doubtful if the Moscow Arts Theatre itself could improve on this production." The second Chichester season the following year consisted of a revival of Uncle Vanya and two new productions—Shaw's Saint Joan and John Arden's The Workhouse Donkey. In 1963 Olivier received another BAFTA nomination for his leading role as a schoolteacher accused of sexually molesting a student in the film Term of Trial.

At around the time the Chichester Festival opened, plans for the creation of the National Theatre were coming to fruition. The British government agreed to release funds for a new building on the South Bank of the Thames. Lord Chandos was appointed chairman of the National Theatre Board in 1962, and in August Olivier accepted its invitation to be the company's first Director. As his assistants, he recruited the Directors John Dexter and william Gaskill, with Kenneth Tynan as literary adviser or "dramaturge". Pending the construction of the new theatre, the company was based at the Old Vic. With the agreement of both organisations, Olivier remained in overall charge of the Chichester Festival during the first three seasons of the National; he used the festivals of 1964 and 1965 to give preliminary runs to plays he hoped to stage at the Old Vic.

Olivier said in 1963 that he believed he was born to be an actor, but his colleague Peter Ustinov disagreed; he commented that although Olivier's great contemporaries were clearly predestined for the stage, "Larry could have been a notable ambassador, a considerable minister, a redoubtable cleric. At his worst, he would have acted the parts more ably than they are usually lived." The Director David Ayliff agreed that acting did not come instinctively to Olivier as it did to his great rivals. He observed, "Ralph was a natural actor, he couldn't stop being a perfect actor; Olivier did it through sheer hard work and determination." The American actor william Redfield had a similar view:

During the following year Olivier concentrated on management, directing one production (The Crucible), taking the comic role of the foppish Tattle in Congreve's Love for Love, and making one film, Bunny Lake is Missing, in which he and Coward were on the same bill for the first time since Private Lives. In 1966, his one play as Director was Juno and the Paycock. The Times commented that the production "restores one's faith in the work as a masterpiece". In the same year Olivier portrayed the Mahdi, opposite Heston as General Gordon, in the film Khartoum.

In 1967 Olivier was caught in the middle of a confrontation between Chandos and Tynan over the latter's proposal to stage Rolf Hochhuth's Soldiers. As the play speculatively depicted Churchill as complicit in the assassination of the Polish prime minister Władysław Sikorski, Chandos regarded it as indefensible. At his urging the board unanimously vetoed the production. Tynan considered resigning over this interference with the management's artistic freedom, but Olivier himself stayed firmly in place, and Tynan also remained. At about this time Olivier began a long struggle against a succession of illnesses. He was treated for prostate cancer and, during rehearsals for his production of Chekhov's Three Sisters he was hospitalised with pneumonia. He recovered enough to take the heavy role of Edgar in Strindberg's The Dance of Death, the finest of all his performances other than in Shakespeare, in Gielgud's view.

Olivier had intended to step down from the directorship of the National Theatre at the end of his first five-year contract, having, he hoped, led the company into its new building. By 1968 because of bureaucratic delays construction work had not even begun, and he agreed to serve for a second five-year term. His next major role, and his last appearance in a Shakespeare play, was as Shylock in The Merchant of Venice, his first appearance in the work. He had intended Guinness or Scofield to play Shylock, but stepped in when neither was available. The production by Jonathan Miller, and Olivier's performance, attracted a wide range of responses. Two different critics reviewed it for The Guardian: one wrote "this is not a role which stretches him, or for which he will be particularly remembered"; the other commented that the performance "ranks as one of his greatest achievements, involving his whole range".

In 1969 Olivier appeared in two war films, portraying military Leaders. He played Field Marshal French in the First World War film Oh! What a Lovely War, for which he won another BAFTA award, followed by Air Chief Marshal Hugh Dowding in Battle of Britain. In June 1970 he became the first actor to be created a peer for services to the theatre. Although he initially declined the honour, Harold Wilson, the incumbent prime minister, wrote to him, then invited him and Plowright to dinner, and persuaded him to accept.

In the mid-1970s Olivier became increasingly involved in television work, a medium of which he was initially dismissive. In 1973 he provided the narration for a 26-episode documentary, The World at War, which chronicled the events of the Second World War, and won a second Emmy Award for Long Day's Journey into Night (1973). In 1975 he won another Emmy for Love Among the Ruins. The following year he appeared in adaptations of Tennessee Williams's Cat on a Hot Tin Roof and Harold Pinter's The Collection. In 1978 he appeared in the film The Boys from Brazil, playing the role of Ezra Lieberman, an ageing Nazi hunter; he received his eleventh Academy Award nomination. Although he did not win the Oscar, he was presented with an Honorary Award for his lifetime achievement.

After this Olivier played three more stage roles: James Tyrone in Eugene O'Neill's Long Day's Journey into Night (1971–72), Antonio in Eduardo de Filippo's Saturday, Sunday, Monday and John Tagg in Trevor Griffiths's The Party (both 1973–74). Among the roles he hoped to play, but could not because of ill-health, was Nathan Detroit in the musical Guys and Dolls. In 1972 he took leave of absence from the National to star opposite Michael Caine in Joseph L. Mankiewicz's film of Anthony Shaffer's Sleuth, which The Illustrated London News considered to be "Olivier at his twinkling, eye-rolling best"; both he and Caine were nominated for the Academy Award for Best Actor, losing to Marlon Brando in The Godfather.

Olivier spent the last 15 years of his life in securing his finances and dealing with deteriorating health, which included thrombosis and dermatomyositis, a degenerative muscle disorder. Professionally, and to provide financial security, he made a series of advertisements for Polaroid cameras in 1972, although he stipulated that they must never be shown in Britain; he also took a number of cameo film roles, which were in "often undistinguished films", according to Billington. Olivier's move from leading parts to supporting and cameo roles came about because his poor health meant he could not get the necessary long insurance for larger parts, with only short engagements in films available.

The last two stage plays Olivier directed were Jean Giradoux's Amphitryon (1971) and Priestley's Eden End (1974). By the time of Eden End, he was no longer Director of the National Theatre; Peter Hall took over on 1 November 1973. The succession was tactlessly handled by the board, and Olivier felt that he had been eased out—although he had declared his intention to go—and that he had not been properly consulted about the choice of successor. The largest of the three theatres within the National's new building was named in his honour, but his only appearance on the stage of the Olivier Theatre was at its official opening by the Queen in October 1976, when he made a speech of welcome, which Hall privately described as the most successful part of the evening.

Olivier's dermatomyositis meant he spent the last three months of 1974 in hospital, and he spent early 1975 slowly recovering and regaining his strength. When strong enough, he was contacted by the Director John Schlesinger, who offered him the role of a Nazi torturer in the 1976 film Marathon Man. Olivier shaved his pate and wore oversized glasses to enlarge the look of his eyes, in a role that the critic David Robinson, writing for The Times, thought was "strongly played", adding that Olivier was "always at his best in roles that call for him to be seedy or nasty or both". Olivier was nominated for the Academy Award for Best Actor in a Supporting Role, and won the Golden Globe of the same category.

Olivier continued working in film into the 1980s, with roles in The Jazz Singer (1980), Inchon (1981), The Bounty (1984) and Wild Geese II (1985). He continued to work in television; in 1981 he appeared as Lord Marchmain in Brideshead Revisited, winning another Emmy, and the following year he received his tenth and last BAFTA nomination in the television adaptation of John Mortimer's stage play A Voyage Round My Father. In 1983 he played his last Shakespearean role as Lear in King Lear, for Granada Television, earning his fifth Emmy. He thought the role of Lear much less demanding than other tragic Shakespearean heroes: "No, Lear is easy. He's like all of us, really: he's just a stupid old fart." When the production was first shown on American television, the critic Steve Vineberg wrote:

During the production of The Prince and the Showgirl, Olivier, Monroe and her husband, the American Playwright Arthur Miller, went to see the English Stage Company's production of John Osborne's Look Back in Anger at the Royal Court. Olivier had seen the play earlier in the run and disliked it, but Miller was convinced that Osborne had talent, and Olivier reconsidered. He was ready for a change of direction; in 1981 he wrote:

In addition to the naming of the National Theatre's largest auditorium in Olivier's honour, he is commemorated in the Laurence Olivier Awards, bestowed annually since 1984 by the Society of West End Theatre. In 1991 Gielgud unveiled a memorial stone commemorating Olivier in Poets' Corner at Westminster Abbey. In 2007, the centenary of Olivier's birth, a life-sized statue of him was unveiled on the South Bank, outside the National Theatre; the same year the BFI held a retrospective season of his film work.

After being ill for the last 22 years of his life, Olivier died of renal failure on 11 July 1989 aged 82 at his home near Steyning, West Sussex. His cremation was held three days later, and a memorial Service was held in Poets' Corner of Westminster Abbey in October that year.

Together with Richardson and Gielgud, Olivier was internationally recognised as one of the "great Trinity of theatrical knights" who dominated the British stage during the middle and later decades of the 20th century. In an obituary tribute in The Times, Bernard Levin wrote, "What we have lost with Laurence Olivier is glory. He reflected it in his greatest roles; indeed he walked clad in it—you could practically see it glowing around him like a nimbus. ... no one will ever play the roles he played as he played them; no one will replace the splendour that he gave his native land with his genius." Billington commented: