Hardy sings in French, English, Italian, German and has two interpretations in Spanish and one in Portuguese. Her recordings in Italian, completed in Paris in 1963 under the production of Ezio Leoni, remain to this day highly acclaimed. In 1963, she represented Monaco in the Eurovision Song Contest, finishing fifth with "L'amour s'en va". In 1963, she was awarded the Grand Prix du Disque from the Académie Charles Cros (see Grand Prix du Disque for French Song).
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, drawn from Françoise Sagan's piece for theatre of that name). She then did three to four performances as singer in some musicarelli in Italy, for example, Questo pazzo, pazzo mondo della canzone in 1965. This same year, Hardy played a minor role as the Mayor's assistant in Clive Donner’s film What's New Pussycat? and then had 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 participated in Grand Prix, a US blockbuster focusing on Formula 1 racing and the lives of the drivers, directed by John Frankenheimer, in which she plays Lisa, the girlfriend of Nino Barlini, a fictional Italian driver. Following this role, Françoise Hardy did not want to make films anymore, but in 1972 she had a cameo role as a hippie in the film Les Colombes (The Doves) by the Québécois filmmaker Jean-Claude Lord. This was her final appearance on the screen apart from in Claude Lelouch’s 1976 film If I Had to Do It All Over Again (Si c’était à refaire), where she appears as a singer performing a song.