In 1962, Dunaway joined the Lincoln Center Repertory Co., and from 1962 through 1967, she appeared in a number of prominent New York productions. Through this work, she met director Otto Preminger, who cast her in his 1967 film Hurry Sundown. In that same year, she also appeared in Bonnie and Clyde, for which she received an Oscar nomination for Best Actress. Dunaway was nominated again for her work in Chinatown before finally winning the Academy Award for her TV mogul role in 1976's Network.
Dunaway also gave memorable performances in Little Big Man, The Eyes of Laura Mars, The Towering Inferno, The Thomas Crown Affair (the 1968 original) and Mommie Dearest (1981).