Carroll's film debut was a supporting role in "Carmen Jones" (1954), as a friend to the sultry lead character played by Dorothy Dandridge. That same year, she was nominated for a Tony Award for Best Featured Actress in a Musical for her role in the Broadway musical, "House of Flowers". A few years later, she played Clara in the film version of George Gershwin's "Porgy and Bess" (1959), but her character's singing parts were dubbed by opera singer Loulie Jean Norman. The following year, Carroll made a guest appearance in the series "Peter Gunn", in the episode "Sing a Song of Murder" (1960). In the next two years, she starred with Sidney Poitier, Paul Newman, and Joanne Woodward in the film "Paris Blues" (1961) and won the 1962 Tony Award for best actress (the first time for a Black woman) for portraying Barbara Woodruff in the Samuel A. Taylor and Richard Rodgers musical "No Strings". Twelve years later, she was nominated for an Academy Award for Best Actress for her starring role alongside James Earl Jones in the film "Claudine" (1974), which part had been written specifically for actress Diana Sands (who had made guest appearances on "Julia" as Carroll's cousin Sara), but shortly before filming was to begin, Sands learned she was terminally ill with cancer. Sands attempted to carry on with the role, but as filming began, she became too ill to continue and recommended her friend Carroll take over the role. Sands died in September 1973, before the film's release in April 1974.