The burst of stardom that accompanied her portrayal led to two of her archetypal ice maiden roles, first in Roman Polanski's terrifying Repulsion in 1965 and then in Buñuel's 1967 Belle de Jour. Deneuve's startling portrayal of an icy, sexually adventurous housewife in the latter film helped to establish her as one of the most remarkable and compelling actresses of her generation. She further demonstrated her talent that year in Demy's Umbrellas musical follow-up, Les Demoiselles de Rochefort, which she starred in with her sister, Françoise Dorléac.

Deneuve continued to work steadily through the 1960s and 1970s in films such as the 1970 Tristana (her second collaboration with Buñuel) and A Slightly Pregnant Man (1973), in which she starred with her lover at the time, Marcello Mastrioanni (who would father her daughter, the actress Chiara Mastrioanni).

Despite or perhaps because of her stardom, Deneuve chose to avoid Hollywood, limiting her appearances in American films to The April Fools (1969) and Hustle (1975). Tellingly, her most significant American screen work of that period was probably the series of commercials she did for Chanel perfume in the mid-'70s, which led to the creation of her own perfume a decade later. Deneuve also did prolific work through the 1980s, appearing in such films as François Truffaut's Le Dernier Métro (1980) and Tony Scott's The Hunger (1983). The latter film saw Deneuve playing a bisexual vampire alongside David Bowie and Susan Sarandon, and her performance won her an indelible cult status in the States among lesbians, goths, and artistically inclined teenage boys.

In the 1990s, Deneuve garnered further international acclaim for her roles in several films, including the 1992 film Indochine (for which she won a French Academy Award and a Best Actress Oscar nomination) and two films directed by André Téchiné in which she played Daniel Auteuil's sister, Ma Saison Préférée (1993) and Les Voleurs (1995). In 1996, she paid homage to the director who had first given her fame by taking part in the documentary L'Univers de Jacques Demy. Closing out the final years of the 1990's Deneuve remained consistantly working in numerous films (in 1999 alone she appeared in no less than six, including director Leos Carax's controversial Pola X) and continuing to turn in compelling performances.

In 2000 Deneuve received much critical attention when cast alongside eccentric Icelandic singer Bjork in the Lars von Trier's melancholy musical Dancer in the Dark. Though it polarized critics and audiences alike, Dancer nevertheless won the Palme d'Or at Cannes Film Festival and continued von Trier's tradition of creating difficult and challanging films that, like them or not, always seem to provoke a strong response.

These days (2006) she spends much of her time gardening at her country house in Normandy. Her life is split between her apartment on the Left Bank in Paris, and Normandy. Her children, Christian, who is 42, and Chiara, 35, are both married and in the film industry.

She recently published a book, a diary called Close Up and Personal, which received mixed reviews.