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Born in Charlotte, North Carolina, 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 again cracked the Billboard Top 40 when he released the self-penned "Let's Work Together (Part 1)" that went to #32 in early 1970 on the Billboard Hot 100. The 1970 hit version was released as a single on Sue Records (Sue 11) and was backed with "Let's Work Together (Part 2)". The song also was released as a 5 minute 19 second song on the Sue Records album SSLP-8801 "Let's Work Together". The song was originally released by Harrison in 1962 as "Let's Stick Together" on Fury 1059 and Fury 1063. "Let's Work Together" would be later be 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', and 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. Harrison was inducted into the North Carolina Music Hall of Fame in 2009.