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Born in Charlotte, North Carolina, United States, Harrison had a Billboard #1 record in 1959 with the song "Kansas City". The song was written in 1952 and was one of the first credited collaborations by the team of Jerry Leiber and Mike Stoller. It sold over one million copies, and was awarded a gold disc. Harrison recorded "Kansas City" for the Harlem based entrepreneur Bobby Robinson.
Harrison recorded for the Fire and Fury record labels, which were owned and operated by Robinson. After this success, Harrison continued to perform and record but it would be another ten years before he recorded "Let's Stick Together" that went to # 32 on the Billboard Hot 100, and a re-worked version titled "Let's Work Together" was later a hit for Canned Heat and Bryan Ferry. It was also recorded by country rock band The Kentucky Headhunters for the soundtrack to the movie, Harley Davidson and the Marlboro Man. In 1970, Harrison had some success with "My Heart Is Yours", and he toured for many years with a band known as 'Wilbert Harrison and The Roamers', as well as a solo act.
In 2001, his recording of "Kansas City" was given a Grammy Hall of Fame Award, and has also been named as one of The Rock and Roll Hall of Fame's 500 Songs that Shaped Rock and Roll. He was inducted into the North Carolina Music Hall of Fame in 2009.