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Sondergaard made her first film appearance in Anthony Adverse as "Faith Paleologue" and became the first recipient of the Oscar for Best Supporting Actress for this performance. Her career as an actress flourished during the 1930s, including a role opposite Paul Muni in Academy Award-winning The Life of Emile Zola.

Walt Disney Studios used her as the main inspiration for the Wicked Queen in the animated film Snow White and the Seven Dwarfs (1937). Originally cast as the Wicked Witch in The Wizard of Oz (1939), she was replaced by Margaret Hamilton when MGM decided to change the Wicked Witch from a glamorous character to an ugly one, and Sondergaard, fearing it could damage her career, refused to wear the necessary disfiguring makeup.

In 1940 she played the role with which she is perhaps most identified, the exotic and sinister wife in The Letter, supporting Bette Davis. She received a second Academy Award nomination as Best Supporting Actress for her role as the King`s wife in Anna and the King of Siam in 1946.

In 1978 Sondegaard played the Dowager Empress Maria Feodorovna in a production of Marcelle Maurette`s play Anastasia at the University of Massachusetts, Amherst.

Married to the film director Herbert Biberman from 1930, her career suffered irreparable damage during the Red Scare of the early 1950s, when her husband was accused of being a communist and named as one of the Hollywood Ten. With her career stalled, she supported her husband during the production of Salt of the Earth (1954). Highly controversial when it was made, and not a commercial success, its artistic and cultural merit was recognized in 1992 when the National Film Preservation Board selected it for preservation in the National Film Registry. The 2000 film One of the Hollywood Ten chronicled Sondergaard`s relationship with Biberman and her role in the making of Salt of the Earth.

Sondergaard and Biberman sold their home in Hollywood shortly after they completed Salt of the Earth, and moved to New York where Sondergaard was able to work in theatre.

Herbert Biberman died in 1971. Sondergaard made a few more film and television appearances, before retiring. She died from cerebral vascular thrombosis in Woodland Hills, California at the age of 86.