Margaret Nolan began her career in front of a camera lens as a model. As her glamour modelling career took off, she was briefly known as Vicky Kennedy in the early 1960s. Nolan reverted to her birth name as soon as acting roles beckoned; appearing in numerous television shows, theatre productions and films. The latter included A Hard Day's Night with the Beatles, Ferry Cross the Mersey with Gerry and the Pacemakers and Marcel Carné's Three Rooms in Manhattan.

In 1964, Nolan played the small role of Dink, Bond's masseuse, in the James Bond film Goldfinger. She was painted gold and wore a gold bikini for Robert Brownjohn's title-sequence, advertisements and soundtrack-cover (not Shirley Eaton as in the narrative of the film). This led to photographs in Playboy magazine's James Bond's Girls edition of November 1965. In the 1971 film Carry On at Your Convenience, Composer Eric Rogers referenced Nolan's Goldfinger affiliation by using its three-note motif on a close-up of her. Nolan appeared on the front cover of both the US and UK versions of the 2005 book Robert Brownjohn: Sex and Typography. The title-sequence was also parodied by the pop-band Scissor Sisters for their 2006 music-video Land of a Thousand Words. In 2012, Nolan gave her first interview concerning her experiences as the model. Asked if the imagery liberates or celebrates womanhood, Nolan responded that

On appearing in Michael Pertwee's 1969 farce She's Done It Again at London's Garrick Theatre, Nolan was described as combining '...a long list of physical attractions with a talent that has contributed to the success of many films and television plays...' She was known for five BBC series with Spike Milligan and in 2013 published a short essay on her time working with him. Nolan gave a live reading of the work at the Poetry Society in Covent Garden, reviewed by What's On London as a "deeply-personal memoir... her performance simply magical." She spoke of her awareness of Milligan's depressive character but also of their friendly working relationship; noting that "Professionally, he taught me that timing is what makes things funny. Timing is crucial..." Nolan was given bigger roles in several 1970s Carry On films – and most sizably Carry On Girls. The scene in Carry On Girls where a woman in a one-piece swim suit sneezes and bursts open two buttons on her outfit (revealing most of her breasts) is Nolan. The same film contains the sequence of Nolan (in a silver bikini) and Barbara Windsor cat-fighting on a hotel floor.

In 2009, early publicity shots of Nolan inspired screen-prints by Brighton-based graffiti Artist Hutch. Nolan's work in photo-montage was also selected for the front cover of Playerist literary magazine (No. 2, 2012). In 2013, her artworks featured in the group show equals: exploring feminism through art and conversation at BLANKSPACE Manchester; the press release quoting that "Her voice carries alongside universal debate on socio-sexual hierarchies in the age of mass media." Nolan lives and works in her home town of Hampstead, continues to exhibit, and occasionally attends conventions for film fans.

Nolan also appeared in serious theatre, motivated by political themes and in one of the first episodes of the television police drama The Sweeney. In 2011, Nolan's work as a comedy Actress was recognised with her name included on Gordon Young's Comedy Carpet installation in front of Blackpool Tower. Also in 2011, Nolan returned to the screen after a gap of nearly three decades. She starred in a role especially written for her by Ann Cameron, in Yvonne Deutschman's The Power of Three. The film was set in Hampstead, and well-received on the independent circuit with a 7.2 rating on IMDb.

It became the first film-title to be shown in installation at MoMA, New York (2012).