Vitouš's virtuoso jazz bass playing has led critics to place him in the same league as Scott LaFaro, Dave Holland, Niels-Henning Ørsted Pedersen and Christian McBride. A representative example of Vitouš's double bass playing is Now He Sings, Now He Sobs (1968), with Chick Corea on piano and Roy Haynes on drums. This album shows his strong rhythmic sense, innovative walking lines, and intensity and abandon as an improviser.
His first album as a leader, Infinite Search, re-released with minor changes as Mountain in the Clouds featured several key figures from the then-budding jazz fusion movement: John McLaughlin, Herbie Hancock, Jack DeJohnette, and (slightly) elder statesman Joe Henderson.
A founding member of the group Weather Report, he has worked with Jan Hammer, Freddie Hubbard, Miles Davis, Chick Corea, Wayne Shorter, Joe Zawinul, and Jan Garbarek. Vitouš has since discussed his contentious departure from Weather Report with journalists, specifically regarding his relationship with Zawinul. Alphonso Johnson, who replaced Vitouš, was himself replaced by the highly innovative and influential bassist Jaco Pastorius. In 1988 Vitouš moved back to Europe to focus on composing, but nonetheless continued to perform in festivals.