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Born Barbara Ann Smith in Smithridge, Louisiana, United States, she was raised in New Orleans and began singing in a church choir. She was discovered by singer Jessie Hill, who recommended her to record producer Harold Battiste. Her first record on Battiste's AFO (All For One) record label, "I Know (You Don't Love Me No More)", which she wrote, was issued in late 1961, and both topped the R&B chart and made number 3 on the Billboard Hot 100 chart. It was later recorded by many other artistes, including Freddie King, Paul Revere & the Raiders (1966), the Merseybeats, Ike and Tina Turner, and Bonnie Raitt (1972).
Two subsequent releases, "You Talk About Love" and "Send For Me (If You Need Some Lovin')", both on AFO, reached the Billboard Hot 100 later in 1962, but failed to match the national success of her first hit.
Later recordings met with more limited success, and George largely retired from the music industry by the late 1960s, with a few subsequent attempts at a comeback being unsuccessful. She sang on the Willy DeVille album, Victory Mixture.