Adderley is remembered for his 1966 soul jazz single "Mercy, Mercy, Mercy", a crossover hit on the pop charts (it was also covered by The Buckinghams). He worked with trumpeter Miles Davis, on his own 1958 Somethin' Else album, and on the seminal Davis records Milestones (1958) and Kind of Blue (1959). He was the older brother of jazz trumpeter Nat Adderley, a longtime member of his band.