Although not a trained or particularly accomplished musician, George Hunter was the driving force behind the formation of the Charlatans, one of the first San Francisco 1960s psychedelic bands. In early 1964 he started to talk about forming a band with Richie Olsen, who ended up as the Charlatans' bassist. Hunter didn't have musical experience, but he had the style and look needed for a far-out new rock band; according to one newspaper account, his hair was "so long it makes the Beatles look like Organization Men." In the Charlatans, he would end up playing tambourine, autoharp, and some rhythm guitar, occasionally singing lead and writing material. The Charlatans barely released anything while Hunter was in the band, but about a couple dozen of 1965-1968 songs on which Hunter plays did surface on the CD collection The Amazing Charlatans. A couple of these were Hunter-Olsen compositions: the sardonically good-time "I Always Wanted a Girl Like You" and the quirkily psychedelic "Walkin'."
The Charlatans disbanded in 1968, and when they re-formed almost immediately (and recorded their sole proper album), the lineup did not include Hunter. Hunter's Globe Propaganda graphic arts company did some San Francisco rock album sleeves for It's a Beautiful Day, Quicksilver Messenger Service, and the Sopwith Camel.