During the summer of 1965 singer Marty Balin recruited folk musician Kantner as part of the original Jefferson Airplane.

During the transitional period of the early 1970s, as the band started to disintegrate, Kantner recorded Blows Against The Empire, a concept album featuring an ad-hoc group of musicians whom he dubbed Jefferson Starship, marking the first-ever use of that name. This edition of Jefferson Starship (such as it was) included members of Crosby, Stills, Nash & Young (David Crosby and Graham Nash) and members of the Grateful Dead (Jerry Garcia, Bill Kreutzman, and Mickey Hart), as well as some of the remaining members of Jefferson Airplane (Slick, Covington, and Casady). In Blows Against the Empire, Kantner (and Slick) sang about a group of people escaping earth in a hijacked starship. In 1971, the album was nominated for the prestigious science fiction prize, the Hugo Award, a rare honor for a musical recording. It was while that album was made that Kantner sealed his love affair with Grace Slick; their daughter China Kantner (who made a name for herself as an MTV veejay in the 1980s) was born shortly thereafter.

Kantner and Slick (with a similar group of musicians, but without a "Jefferson Starship" artist credit) released two follow-up albums: Sunfighter, an environmentalism-tinged album released in 1971 to celebrate China's birth, and 1973's Baron von Tollbooth & the Chrome Nun, titled after the nicknames David Crosby had given to the couple. The artist credit on Baron von Tollboth gave ex-Quicksilver Messenger Service bassist-keyboard player-vocalist David Freiberg equal billing with Kantner and Slick. (Freiberg, who had also appeared on Blows Against the Empire, had joined Jefferson Airplane in time to appear on Thirty Seconds over Winterland.)

Kantner is also credited with discovering teen-age guitarist Craig Chaquico during this time, who first appeared on Sunfighter and would play with Kantner, Slick and their bands and then with Starship through 1991. He later embarked on a successful solo career as a smooth jazz artist.

By 1973, with Kaukonen and Casady now devoting their full attention to Hot Tuna, the musicians on Baron von Tollbooth formed the core of a new Airplane lineup that was formally reborn as Jefferson Starship in 1974. Kantner, Slick, and Freiberg were charter members. The line-up also included late-Airplane holdovers drummer John Barbata, and fiddler Papa John Creach (who also played with Hot Tuna), along with Pete Sears (who, like Freiberg, played bass and keyboards) and twenty-year-old guitarist Craig Chaquico. Although Balin was originally not among the re-christened Jefferson Starship, he joined the band while their first album, Dragonfly, was still in the works.

In 1984, Kantner (the last founding member of Jefferson Airplane remaining) left the group, but not before taking legal action against his former bandmates over the Jefferson name (the rest of the band wanted to continue as Jefferson Starship). Kantner won his suit, and the group name was reduced to simply Starship, marking the third incarnation of the band.

In 1985, following his departure from Jefferson Starship, Paul Kantner rejoined with Balin and Jack Casady to form the KBC Band, releasing their only album, KBC Band (which included Kantner's hit, "America"), in 1987 on Arista Records.

With Kantner reunited with Balin and Casady, the KBC Band opened the door to a full-blown Jefferson Airplane reunion. In 1989, during a solo San Francisco gig, Paul Kantner found himself joined by former bandmate (and lover) Grace Slick and two other ex-Airplane members for a cameo appearance. This led to a formal reunion of the original Jefferson Airplane (featuring nearly all the main members, including founder Marty Balin, but without Spencer Dryden, who had been kicked out of the band years earlier). A self-titled album was released by Columbia Records. The accompanying tour was a success, but their revival was short-lived, and thus Jefferson Airplane was officially disbanded for good.