His early work blends non-western instruments with 1960s folk revival, and has been cited as important in the development of psychedelic music.

An arrangement of Carl Orff's composition Carmina Burana for 5-string banjo appears on his first album and other musical fusions include his adaptation of Luiz Bonfá's "Manhã de Carnaval", a lengthy variation on "Memphis, Tennessee" by Chuck Berry, and compositions derived from works of J. S. Bach and Roebuck Staples.

As documented in the Still Valentine's Day, 1969: Live At the Matrix, San Francisco recording, Sandy Bull's use of tape accompaniment was part of his solo performances in concert as well.

By the 1970s he had relocated to San Francisco, where he shared living and rehearsal space with folk singer Billy Roberts, the composer of the Jimi Hendrix song, "Hey Joe".

On May 2, 1976 he opened a concert by Leo Kottke at the Berkeley Community Theater, where he performed using his 4-track recorder and a 'Rhythm Ace' as backup instruments.