Born Martyn Jerel Buchwald in Cincinnati, OH, Balin moved with his parents to the Bay Area at an early age. He grew up in San Francisco, and after attending college there, changed his name to Marty Balin and began a career as a folk singer.

He recorded two unnoticed albums before forming Jefferson Airplane in 1965 with friend Paul Kantner as one of the earliest folk-rock bands. The group was signed to RCA, and before they made their second album, they recruited vocalist Grace Slick.

After they scored a massive hit with two songs Slick contributed ("Somebody To Love" and "White Rabbit"), Jefferson Airplane became one of the cornerstone acts that launched the youth and drug movements of the 1960s. Balin was critical of the band's musical direction and image, and ego clashes with Kantner finally forced him to leave the band in 1971. He would later rejoin them in the re-named Jefferson Starship in 1974. After contributing many of the hits that took the Starship to the top of the charts, Balin again saw the writing on the wall, and left when they were at the height of their career.