She is well known for her first acting role, appearing opposite her husband, actor Alain Delon, in the neo-noir film Le Samouraï directed by Jean-Pierre Melville (1967).

[5] She was the daughter of Louis Canovas (1915–2003), pied-noir of Oran (Algeria), manager of a transport company in Morocco, who abandoned the family when she was 8 months old in 1942[6] and Antoinette Rodriguez, who was from Melilla.

In August 1962, Nathalie met French actor Alain Delon at New Jimmy's, a Paris nightclub, and they began a secret relationship that night that lasted one year.

During the 1960s and 1970s she dated Bobby Keys, Marc Porel, Eddie Fisher, Renaud Verley, Louis Malle, and Franco Nero, among others.

[5] Writing of the Delons' performances in Le Figaro, Bertrand Guyard notes husband and wife are both nearly silent but "their gazes, fraught with meaning, are enough to thrill the camera" with the director drawing from their portrayals "a mythical couple in the seventh art.

In 1973, she acted in Le Sex Shop, and her role was one of the film's "moments of real pleasure, as one of its "really marvelous girls", commented Roger Greenspun in The New York Times.

[14] In addition to acting in 30 films during her career, she directed two: one was the story—also written by Delon—of a mother whose son dies in surgery, Ils appellent ça un accident [fr] (transl.