After singing in various gospel groups he became a member of The Larks before recording with his wife Anna Lee "Little Ann" Sandford, and then as a solo performer.

[3][4] Eventually settling on the name The Larks, the group's recording of "Eyesight to the Blind" on the Apollo label, with lead vocals and guitar by Bunn, reached number 5 on the Billboard R&B chart in July 1951; and the follow-up, "Little Side Car", also sung by Bunn, reached number 10 on the R&B chart later the same year.

[2] Bunn returned to solo recording, using the name Tarheel Slim, in New York in 1958, for producer Bobby Robinson's Fury label.

His first recordings for Fury, "Wildcat Tamer" / "Number 9 Train", have been described by AllMusic critic Bill Dahl as "a pair of rockabilly raveups",[4] and by another reviewer as "pinnacles of New York rock'n'roll".

[2] In the early 1970s, Tarheel Slim was "rediscovered" by researcher Peter Lowry, and emerged to play solo, with acoustic guitar in the style of Brownie McGhee, at festivals and for college audiences.