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Born Barbara Ann Smith at Charity Hospital in New Orleans, Louisiana, United States, she was raised in the 9th ward New Orleans, Louisiana 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 her mother Eula Mae Jackson 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 such as the 1979 Senator Jones produced "Take Me Somewhere Tonight", met with more limited success, and George largely retired from the music industry by the early 1980s, with subsequent singles never achieving the success of the Harold Battiste produced, and certified gold single, "I Know". She sang on the Willy DeVille album, Victory Mixture.
Barbara gave birth to three sons, Tevin, Albert and Gregory. Barbara's son Tevin George trained as a professional boxer and is listed as the United States 1986 winner of the Golden Gloves award subsequently going on to perform in the Olympic Trials.