Hardy remains a popular figure in music and fashion, and is considered an icon of French pop and the 1960s.

After a year at the Sorbonne she answered a newspaper advertisement looking for young Singers. Hardy signed her first contract with the record label Vogue in November 1961. In April 1962, shortly after she left university, her first record "Oh Oh Chéri" appeared, written by Johnny Hallyday's writing duo. Her own flip side of the record, "Tous les garçons et les filles" became a success, riding the wave of Yé-yé music in France. It sold over a million copies, and was awarded a gold disc. The track peaked at No. 36 in the UK Singles Chart in 1964. She reportedly hated the song saying it was recorded "in three hours with the worst four Musicians in Paris." She was dating Photographer Jean-Marie Périer at this time and his shots featured on many of her record sleeves.

Françoise Hardy made her film debut in 1963, after having been chosen by Director Roger Vadim to take the role of Ophélie in his movie Nutty, Naughty Chateau (Château en Suède), according to Françoise Sagan's play. She then did three to four performances as singer in some musicarelli in Italy as for example: Questo pazzo, pazzo mondo della canzone in 1965. This same year, Hardy also played a minor role as the Mayor's assistant in Clive Donner’s film What's New Pussycat? and then held a supporting role in A Bullet Through the Heart (Une balle au cœur), directed by Jean-Daniel Pollet. In 1966, she made a cameo appearance in a scene from Jean-Luc Godard's film Masculin, féminin then participate in Grand Prix, a US blockbuster on racing of Formula 1, directed by John Frankenheimer, in which she is Lisa, the girlfriend of Nino Barlini, a fictional Italian driver. After this film, Françoise Hardy does not want to make a cinema anymore but in 1972 she plays a hippie; just one cameo for the film, Les Colombes (The Doves), by the Québécois filmmaker, Jean-Claude Lord. This will be her last appearance on the screens if not that of 1976 in Claude Lelouch’s film If I Had to Do It All Over Again (Si c’était à refaire), where she appears in her role of singer to interpret just one song.

Hardy is mentioned in a poem by Bob Dylan, "Some other kinds of songs", which appears on the back cover of his album Another Side of Bob Dylan, released in 1964.

In a scene from Director John G. Avildsen's film Save the Tiger (1973), Jack Lemmon's character Harry Stoner makes a reference to Hardy during a melancholy telephone call to his wife. Her song "Tous les garçons et les filles" played during the British film Metroland (1997) and Bernardo Bertolucci's The Dreamers (2003). The French movie 8 Femmes (2002) features her song "Message Personnel" as sung by the French Actress Isabelle Huppert. Her recording of "Träume" plays during the end credits of François Ozon's Water Drops on Burning Rocks (Gouttes d'eau sur pierres brûlantes) (2000). Her song "L'Amitié" is played during the end credits of Denys Arcand's movie The Barbarian Invasions (Les Invasions barbares) which won the Academy Award for Best Foreign Language Film in 2003 (the main character had referenced her in an earlier scene in the movie with images dating from 1965).

In 1981, she married her long-time partner Jacques Dutronc, who is the father of her son, Thomas Dutronc, born in 1973. Hardy lives in the 16th arrondissement of Paris and Dutronc in Monticello, Corsica, although they reportedly remain legally married.

In 1994, she collaborated with the British pop group Blur for their "La Comedie" version of "To the End". In 1995, she sang on Malcolm McLaren's single "Revenge of the Flowers". The song appears on his concept album Paris. In May 2000, she made a comeback with the album Clair-obscur on which her son played guitar and her husband sang the duet "Puisque vous partez en voyage". Iggy Pop and Étienne Daho also took part. She has also recorded a duet with Perry Blake who wrote two songs for Tant de belles choses. For this album, Hardy won the trophy "Female Artist of the Year" at the Victoires de la musique ceremony in 2005.

Her recording of the song "Il n'y a pas d'amour heureux", composed by Louis Aragon, is played in the Norwegian film Tatt av Kvinnen (2007). In the award-winning Greek film Attenberg (2010), her song "Tous les garçons et les filles" is played and sung by the two main characters in a lament of adolescent longing and loneliness.

In Wes Anderson's Moonrise Kingdom (2012), her song "Le temps de l'amour" features prominently. The film's two lead characters, a pair of 12-year-old runaways, dance on the beach and have a romantic interlude as the song plays on a portable turntable. The female lead (Suzy) calls The "Yeh-Yeh" Girl from Paris! (1962) her "favorite record album", and it is the only album she packs when preparing to run away from home.

Because of her difficult upbringing Hardy became painfully shy – a trait which is still part of her character today. When asked about her shyness in an interview with John Andrew, broadcast on BBC Radio 4 in 2011 she said:

Hardy's song "Ce Petit Cœur", was featured in the Gilmore Girls episode "French Twist". Her song "Ma jeunesse fout le camp" was also played in the television series La Femme Nikita's third season episode "Beyond the Pale" when Nikita pulls out an old record and plays the song. "Le Temps de l'amour" featured in the closing sequence of the first season finale of Helix. Her song "All Because of You" was covered by Jessica Sula and appeared in the first episode of the sixth season of Skins. Sula's character, Grace Blood, covered the song to submit as her music final in college, but wasn't able to finish it due to a fatal car accident. "Tous les garçons et les filles" also appeared in the final episode of the 2015 British mini-series The Enfield Haunting. Her song "Voilà" appears in the British television series The End of the F***ing World.