His first album in the U.S., Prelude, released in 1972, was of a big band Latin jazz style that immediately attracted a wide audience. The album was produced by Creed Taylor on his CTI (Creed Taylor Inc.) label. The nine-minute funky version of Richard Strauss' Also Sprach Zarathustra, entitled "Also Sprach Zarathustra (2001)", won the 1974 Grammy Award for Best Pop Instrumental Performance. It went to No. 2 in the pop charts in the US, No. 3 in Canada, and No. 7 in the UK and was CTI's biggest single. The album climbed to No. 3 in the Billboard chart, the label's best-selling album and an amazing sales achievement for a jazz-based release. It was subsequently used to great effect in the 1979 film Being There, starring Peter Sellers and Shirley MacLaine. It has also been covered extensively by the rock band Phish in their live performances and included in several of their live releases.
His second album, Deodato 2, despite being of the same style and quality, failed to sell as well, but climbed to number 19 in the Billboard album chart, whilst the single, "Rhapsody In Blue" reached No. 41 on the Hot 100 in 1973. Another track from the album, his interpretation of Ravel's "Pavane pour une infante defunte" ("Pavane for a Dead Princess"), was used for a number of years in the 1970s by the Australian Broadcasting Corporation's television station ABN-2 in Sydney, serving as the background music for a videotaped sequence of scenes of Sydney at night, which marked the end of transmission for the day (in the period before the ABC commenced 24-hour broadcasting).
His early career records used guitarist John Tropea and quintessential jazz fusion flautist Hubert Laws. He was also known for utilizing the signature funky electric piano sound of the Fender Rhodes, specifically with his trademark gritty tube drive. Deodato continued recording until the late 1980s on the Warner Bros label, but never reached the level of his early successes, although two singles, "S.O.S., Fire In The Sky" and "Are You For Real", were Top 20 Billboard Dance hits in 1985.