Moore was an integral part of the Nat King Cole Trio during 1937–1947, appearing on virtually all of Cole's records during the period. A superb and influential guitarist, Moore was himself influenced by Charlie Christian. Barney Kessel once said that Moore practically created the role of the jazz guitarist in small combos. He also recorded with Lionel Hampton, Art Tatum (1941), the Capitol Jazzmen, and Lester Young.
Unfortunately, Moore's post-Cole career was not very successful. He played with his brother Johnny Moore in the Three Blazers from 1947 to the mid-1950s, after which the group declined in popularity following the departure of pianist/singer Charles Brown. Moore also recorded three records for the Verve and Tampa labels during 1953 and 1954. After that he was outside of music with the exception of one Cole tribute album in 1965. Eventually he left music altogether and settled in Los Angeles, where he worked as a bricklayer.