According to The Guardian, the very best Audrey Hepburn film is "Charade". Released in 1963, the film is a Hitchcock-style thriller set in Paris and focuses on Hepburn's character Regina, who is being tracked down by money-chasing thugs. She is eventually saved by her love interest Peter, played by Cary Grant. The film is a romantic thriller with elements of comedy, and Hepburn is a star throughout, wearing plenty of jewels and Givenchy as she flees for her life. The BFI, aka British Film Institute, also ranks "Charade" high on the list of their essential viewing Audrey Hepburn films, calling the chemistry between Grant and Hepburn "exquisite."

However, the film that catapulted Hepburn to fame is undoubted "Roman Holiday," which was released 10 years earlier. The Guardian ranks this film fourth, noting that the director William Wyler called Hepburn "absolutely enchanting" when she auditioned. Moreover, Vogue France puts "Roman Holiday" at the top of their list. Hepburn's role in "Roman Holiday" also won the actress her first and only Oscar for Best Actress, making this film an especially meaningful choice.