In 1931 she went to Hollywood, where she appeared in several films, in small roles. In 1932, she met Charlie Chaplin, and they became a couple shortly afterwards. They married in 1936 and divorced in 1942. He cast her in Modern Times, but it wasn't until they separated, and she got a starring role in The Women, that she became a star (although she had been considered for the role of Scarlett O'Hara in Gone With the Wind).
She starred in The Great Dictator (with Chaplin), Reap the Wild Wind and The Diary of a Chambermaid (with Burgess Meredith, whom she eventually married). She was nominated for the Academy Award for Best Supporting Actress in 1943 for So Proudly We Hail, but her career faded in the 1950s, and she eventually moved to Europe.
In 1958 Goddard married Erich Maria Remarque. They remained married until his death in 1970. Goddard settled in Switzerland, where she eventually died. In her will, she left $20 million to New York University.
There has been much speculation as to Goddard's age. Actress Claire Trevor, who was born in 1910, went to school with her, and claimed that she was a year older than Trevor.