For audiences in the 1940s and 50s, Louis Jourdan’s incredible good looks and mellifluous Gallic purr seemed to sum up everything that was sexy and enticing about Frenchmen. As a result, he became the most sought-after French actor since Charles Boyer. Though perhaps this hampered him, stymying opportunities to extend his dramatic range, any actor who was constantly in demand by both French studios and Hollywood producers had a lot to be grateful for.

When Jourdan, who has died aged 93, played the consummate bon vivant in Vincente Minnelli’s Gigi (1958), he became an international celebrity. The film, which co-starred Maurice Chevalier and Leslie Caron, won nine Oscars, including best picture. Though the best-known of its Lerner and Loewe numbers was Chevalier’s Thank Heaven for Little Girls, the title song went to Jourdan. He later widened the breadth of his work, and in old age was still one of the most handsome men on the screen, even if the films themselves seldom amounted to much.

He was born in Marseille, one of the three sons of Henri Gendre, a hotelier who organised the Cannes film festival after the second world war, and Yvonne, from whose maiden name, Jourdan, Louis took his stage name. The family followed Henri’s work, which accounted for the ease with which he was later able to perform overseas. He was educated in France, Turkey and Britain, where he learned to speak perfect English with an accent that he was clever enough to realise he should keep superbly French.

Jourdan, who knew from early on that he was going to be an actor, studied under René Simon in Paris. Admired for his dramatic talent and a certain polish that no one could readily explain, he was cast in his film debut, Le Corsaire (1939), which starred Boyer, though the outbreak of the second world war prevented its completion. He went on to appear in L’Arlésienne (1942) before his career was interrupted by the Nazi occupation of France.

His father was arrested by the Gestapo, and Louis and his two brothers were active members of the resistance, whose work for the underground meant that he had to stay away from the studios. But it also resulted in his becoming a favourite of the resurgent French postwar film industry. At a time when many had worked on films that had served to help Marshal Pétain’s propaganda campaign – and stars such as Chevalier were being accused of collaboration – it was easy to promote a star who had actively worked against the Nazis.

In 1946, Jourdan married Berthe Frédérique (known as Quique) and went to Los Angeles, having been persuaded by the movie mogul David O Selznick that he would be able to make more of himself in Hollywood than he ever could in Paris. He shone in his first American film, The Paradine Case (1947), directed by Alfred Hitchcock and starring Gregory Peck. This was followed by Max Ophüls’s masterly Letter from an Unknown Woman (1948), based on the story by Stefan Zweig. Jourdan played the debonair, womanising pianist with whom Joan Fontaine falls hopelessly and tragically in love. He invested the performance with a vulnerability that saved his character from being simply caddish.

In Minnelli’s 1949 film of Gustave Flaubert’s Madame Bovary, he starred as the lover of the adulterous anti-heroine, played by Jennifer Jones. He returned to France for Rue de l’Estrapade (1953) and La Mariée Est Trop Belle (The Bride Is Too Beautiful, released with the title Her Bridal Night, 1956), the latter with Brigitte Bardot, while in Italy he appeared in Three Coins in the Fountain (1954), its title referring to the Trevi fountain in Rome. His image as the light romantic lead was burnished in that film, and his status as such was sealed by Gigi, which made him the No 1 pin-up of sophisticated American women.

He had a similar role in Can-Can (1960), which starred Frank Sinatra, Shirley MacLaine and Chevalier. There followed continental roles in Hollywood productions: as a playboy in The VIPs (1963) and a fashion designer in Made in Paris (1966).

He had made his Broadway debut, playing a repressed gay man embarking on marriage, in an adaptation of André Gide’s The Immoralist, in 1954. The production co-starred Geraldine Page and James Dean, before Dean’s movie breakthrough. The following year, Jourdan returned to the New York stage in Tonight in Samarkand. He soon let it be known that he wanted more serious film roles and was not getting enough of them. In 1961 he took the lead in Claude Autant-Lara’s Le Comte de Monte Cristo and, in 1975, he appeared in a British TV movie production of Alexandre Dumas’s novel, this time playing De Villefort to Richard Chamberlain’s Count. Two years later, he was D’Artagnan in The Man in the Iron Mask on TV, again opposite Chamberlain.

He played Dracula in a 1977 BBC TV adaptation and a “charming” villain, Kamal Khan, in the James Bond adventure Octopussy (1983), but few of his later roles showed the range of his talents. Certainly, Swamp Thing (1982) and The Return of Swamp Thing (1989) were not the sort of movies that the Gigi star would want to be remembered for. In the mid-80s he returned to Gigi, this time in Chevalier’s role, for a touring show; he replied to the criticism that he lip-synched songs by saying: “If I sang them live, the fragile little voice I have would go.”

Jourdan’s final film appearance came as a suave villain in Peter Yates’s caper about a rare bottle of wine, Year of the Comet (1992). In 2010 he was appointed to the Légion d’Honneur.

His wife died last year. Their son, Louis Henry, died in 1981 from a drug overdose. He is survived by a nephew and a niece.

• Louis Jourdan (Louis Robert Gendre), actor, born 19 June 1921; died 14 February 2015

• This article was amended on 16 February 2015. Louis Jourdan was born in June 1921 rather than 1919, and so died at the age of 93.