In the early 1930s, she moved to Hollywood and gained notice as the romantic partner of actor and comedian Charlie Chaplin, appearing as his leading lady in Modern Times (1936) and The Great Dictator (1940).

After signing with Paramount Pictures, Goddard became one of the studio's biggest stars with roles in The Cat and the Canary (1939) with Bob Hope, The Women (1939) with Joan Crawford, North West Mounted Police (1940) with Gary Cooper, Reap the Wild Wind (1942) with John Wayne and Susan Hayward, So Proudly We Hail!

[11] Her marriages to Chaplin, the actor Burgess Meredith, and the writer Erich Maria Remarque received substantial media attention.

According to Goddard, her father left them, but according to J. R. Le Vee, Alta absconded with the child to avoid a custody battle, she and her mother moved often during her childhood, including relocating to Canada at one point.

An important figure in her childhood was her mother's paternal uncle Charles Goddard, the owner of the American Druggists Syndicate.

[15] Ziegfeld hired her for another musical, Rio Rita, which opened in February 1927, but she left the show after only three weeks to appear in the play The Unconquerable Male, produced by Archie Selwyn.

She also appeared in City Streets (1931), Ladies of the Big House (1931), and The Girl Habit (1931) for Paramount, Palmy Days (1931) for Goldwyn, and The Mouthpiece (1932) for Warners.

However, Goddard and Goldwyn did not get along, and she also began work for Hal Roach Studios in 1932, appearing in a string of uncredited supporting roles for the next four years.

[18] The year she signed with Hal Roach, Goddard began dating Charlie Chaplin, a relationship that received substantial attention from the press.

"[20] It marked a turning point in Goddard's career when Chaplin cast her as his leading lady in his next box office hit, Modern Times (1936).

Her role as "The Gamin," an orphan girl who runs away from the authorities and becomes The Tramp's companion, was her first credited film appearance and garnered her mainly positive reviews, Frank S. Nugent of The New York Times describing her as "the fitting recipient of the great Charlot's championship".

However, Chaplin worked on his projects slowly, and Goddard worried that the public might forget about her if she did not continue to make regular film appearances.

Initial screen tests convinced Selznick and director George Cukor that Goddard would require coaching to be effective in the role, but that she showed the most promise.

Notably, the head of Selznick's publicity department Russell Birdwell had strong misgivings about Goddard, writing, "Briefly, I think she is dynamite that will explode in our very faces if she is given the part.

"[23] In 1939, Goddard signed a contract with Paramount Pictures and was promptly teamed with comedian Bob Hope for the horror comedy film The Cat and the Canary (1939).

She was also cast for the musical comedy Second Chorus opposite Fred Astaire, Artie Shaw, and future husband Burgess Meredith.

[citation needed] In 1940, Goddard made the Cecil B. DeMille Western film North West Mounted Police opposite Gary Cooper and Madeleine Carroll.

Her other film for 1941, romantic drama Hold Back the Dawn with Charles Boyer and Olivia de Havilland, received positive reviews.

In 1942, Goddard gave one of her better-remembered film appearances in the variety musical Star Spangled Rhythm, in which she sang "A Sweater, a Sarong, and a Peekaboo Bang" with Dorothy Lamour and Veronica Lake.

Their third film, The Crystal Ball, was bought by United Artists – a studio co-founded by Chaplin – and released the following year to tepid box office receipts.

In 1947, she starred in two box office disasters: the historical epic Unconquered, which reunited her with Cooper and DeMille; and the comedy An Ideal Husband, which she made in Britain for Alexander Korda.

Although one of the year's highest-grossing films, Unconquered had a large budget – further inflated by going past its shooting schedule – that caused it to lose money for Paramount.

An Ideal Husband suffered from behind-the-scenes difficulties that included a crew strike over Goddard using her personal, Swedish-born hairdresser over an English one.

Wealthy from shrewd investments, she largely retired from acting and moved with him to Ronco sopra Ascona, Switzerland, where she lived with Remarque in his villa Casa Monte Tabor.

She also became a fairly well known and highly visible socialite in New York City, appearing covered with jewels at many high-profile cultural functions with several well-known men, including Andy Warhol, with whom she sustained a friendship for many years until his death in 1987.

[35] Goddard married the much older lumber tycoon Edgar James on June 28, 1927, when she was 17 years old; the couple moved to North Carolina.