He finally began composing his material with The Time Machine (april 1966), that featured bassist Steve Swallow, Tennessee Firebird (september 1966) attempted a fusion of jazz and country music, even featuring Chet Atkins. In 1967 Burton, who had already experimented with the rhythms of rock music, formed a quartet with guitarist Larry Coryell, Swallow and drummer Roy Haynes, that recorded the first jazz-rock album, Duster (april 1967), highlighted by mesmerizing Coryell playing, followed by Lofty Fake Anagram (august 1967). After performing Carla Bley's composition A Genuine Tong Funeral (1967), Burton came full circle by adding country music to the mix on Country Roads and Other Places (september 1968), recorded by a new quartet that simply replaced Coryell with guitarist Jerry Hahn, and on Throb (june 1969), added country violinist Richard Greene to that quartet. And then Burton embraced electronic keyboards for Good Vibes (september 1969), which was basically a rhythm'n'blues album. Alone at Last (june 1971) experimented with overdubbing various keyboards and with the solo vibraphone format. The problem with all of Burton's visionary experiments is that the material was of extremely poor quality (mostly covers).

Then Burton decisively joined the jazz-rock bandwagon. After Gary Burton & Keith Jarrett (july 1970), that had a quintet almost entirely devoted to Jarrett compositions, and Crystal Silence (november 1972), a collaboration with Corea that, again, mainly belonged to the pianist, Burton formed a New Quartet (march 1973) but continued to play other people's music with little or no personality. Burton inaugurated a quintet with guitarists Mick Goodrick and Pat Metheney, bassists Steve Swallow and drummer Bob Moses on Ring (july 1974), also featuring bassist and jazz-rock star Eberhard Weber, and Dreams So Real (december 1975), devoted to Carla Bley material (without Weber). Even better was Passengers (november 1976), with the same duo of bassists but only one guitarist (Metheny) and Dan Gottlieb on drums. Yet another edition of the quartet, with Swallow, Haynes and Japanese trumpeter Tiger Okoshi, debuted on Times Square (january 1978) Permutations of the quartet continued stoically. Real Life Hits (november 1984) had Japanese pianist Makoto Ozone. Whiz Kids (june 1986) added British saxophonist Tommy Smith to the quartet. The quartet of Times Like These (september 1988) boasted guitarist John Scofield, bassist Marc Johnson and drummer Peter Erskine. Departure (march 1997) wasted Scofield, Erskine, pianist Fred Hersch and bassist John Patitucci on the usual program of poppish material. For Hamp, Red, Bags, and Cal (june 2000) was a tribute to the great vibraphonists of jazz. The quintet of Generations (september 2003) and Next Generation (november 2004) was perhaps the least inspired group of his career.

The Gary Burton Quartet with Jim Odgren (alto sax), Steve Swallow (bass) and Mike Hyman (drums) recorded Picture This (january 1982), devoted to compositions by Odgren and covers of Michael Gibbs, Chick Corea, Carla Bley and Charlie Mingus.