With this lineup the group would have a series of hits between 1959 and 1964 and participated on many of the albums that helped to bring R&B to a crossover audience, including the landmark million-selling 1963 live album, Live at the Apollo. Byrd and the Famous Flames also performed together on a few episodes of The Ed Sullivan Show, made a brief appearance in the film, Ski Party and upstaged headliners The Rolling Stones on the landmark 1964 rock concert/motion picture, The T.A.M.I. Show. Byrd (and fellow Famous Flame Lloyd Stallworth) were credited as songwriters on the Flames hit, "Lost Someone," though Brown was the only member who sang on the recording. Its success led Brown to record more songs on his own but the majority of his early hits were as a member of the Famous Flames including songs such as "Try Me", "I'll Go Crazy", "Bewildered", "Think", "Baby You're Right", "I Don't Mind", "This Old Heart", "Shout and Shimmy", and "Oh Baby Don't You Weep". As was the case with some recordings, the Famous Flames were often not credited on album covers though ironically enough on recordings in which Brown appeared by himself, the group was credited, leaving fans to erroneously believe the Famous Flames were actually Brown's backing band, instead of the singing group that they actually were. The group continued performing together until 1968 when they left over monetary issues. The last Flames-associated recording to be released was the pre-funk soul hit, "Licking Stick - Licking Stick", to which Byrd contributed vocals without the other members, who had departed before Byrd did that summer.
When The Famous Flames were still together, Byrd and Brown co-formed the production company, Fair Deal, to distribute The Famous Flames' recordings – and Brown's own solo recordings – to mainstream markets after years solely on the rhythm and blues circuit. This led to both Byrd and Brown's signing solo deals with Smash Records. In 1964, Byrd recorded his first solo hit, "Baby, Baby, Baby" with Anna King. A year later he had a bigger R&B hit with "We Are in Love", which reached #14. Later in the late 1960s, as Byrd and Brown together began working under the yet-to-be-named genre of funk, Byrd had a funky song "I Need Help (I Can't Do It Alone)"(1970).