Graham Bond was educated at the prestigious Royal Liberty School in Gidea Park, East London. He first gained attention as a jazz saxophonist as a member of the Don Rendell Quintet. Afterwards, he was briefly a member of Blues Incorporated, a group led by Alexis Korner, before forming the Graham Bond Quartet. With a lineup of Bond on vocals and organ, Ginger Baker on drums, Jack Bruce on double bass, and, briefly, John McLaughlin on guitar, who was replaced by Dick Heckstall-Smith on sax and the name changed to the Graham Bond Organization (GBO), they generally stayed close to their jazz and R&B roots. Bond was the primary songwriter, and he also produced the group's two studio albums, The Sound of '65 and There's a Bond Between Us.

The GBO is notable in popular music history for jump-starting the careers of two future Cream members, bassist/singer Jack Bruce and drummer Ginger Baker. One song Bruce and Baker originally recorded with Bond, "Train Time," later wound up in the repertoire of Cream.

Later when blues and R&B scenes erupted on the British gig circuit, the Graham Bond Organization became known for playing the most evil-sounding and dirty R&B heard in England. When Jack Bruce and Ginger Baker left the band, Jon Hiseman joined the GBO.

In a sense, Bond was a catalyst in the formation of British groups Cream and Colosseum, as members of those groups came from Bond's group. Although highly influential within English music circles, the GBO never experienced the popular chart success of their peers.

One factor for this could have been Bond's rough, growling singing voice, which was an acquired taste. Another was the decided lack of conventional star appeal of the four members: Bond, Bruce, Baker, and saxophonist Dick Heckstall-Smith.

In addition, the group's studio albums were never released in the United States. Bruce, then Baker left the band to form Cream in July 1966.

Amid internal band struggles and Bond's worsening problems with substance abuse, the GBO disbanded in 1967.