Carroll's first brush with celebrity was when she was the model for The Spirit of the Centennial statue at the 1936 Texas Centennial Exposition at Fair Park in Dallas, Texas. The statue still stands in front of what is now The Women's Museum. She is a 1937 graduate of Woodrow Wilson High School in Dallas and has been inducted into the school's Hall of Fame, which is chock-full of distinguished graduates.
Carroll's acting career began in 1941 when she appeared in several uncredited small roles in films such as Maisie Was a Lady with Lew Ayres and Ann Sothern, Ziegfeld Girl with Judy Garland, as well as You're in the Army Now and Navy Blues, in both of which she appeared with the Navy Blues Sextette group.
Possibly her most visible acting role was as Betsy Ross in the James Cagney musical Yankee Doodle Dandy in 1942. She also did modelling during this time, appearing in advertisements for Jewelite hairbrushes, among other products.
In 1943, Carroll joined Kay Kyser's band, known as the Kollege of Musical Knowledge, as a featured vocalist. Capitalizing on her good looks, she was given the nickname Gorgeous Georgia Carroll, probably as a joking reference to the professional wrestler George Wagner, who used the name Gorgeous George. As a member of Kyser's band, Carroll appeared in three films: Around the World, Carolina Blues, and most notably the Second World War-era morale booster Thousands Cheer which gave fans a chance to see Kyser and his band in Technicolor. Kyser's band has a featured performance near the end of the film, with Carroll delivering a key solo interlude of the Arthur Freed/Nacio Herb Brown standard, Should I?