In 1985, Brook made his solo debut with Hybrid, an influential ethno-ambient work recorded with Eno that explored the middle ground between Western and Indian musical aesthetics and established his unique, heavily processed "infinite guitar" sound. He spent much of the remaining decade working with Eno, helping create video sculptures and sound installations across the globe; he also became a sought-after producer, helming records for such diverse talents as Roger Eno, Pieter Nooten, Mary Margaret O'Hara, Balloon, and the Pogues. In 1990, Brook returned to world music, producing Youssou N'Dour's acclaimed Set; more importantly, he began a continuing collaboration with Pakistani qawaali singer Nusrat Fateh Ali Khan with the seminal Mustt Mustt, a fusion of Western ambient and pop sounds with the sacred spiritual music of the East.

After producing Khaled, a 1991 project for the Algerian rai vocalist Cheb Khaled, Brook returned to the studio to record his first solo effort in seven years, 1992's stellar Cobalt Blue. A rare concert performance given at a party celebrating the album's release was subsequently issued as the limited-edition Live at the Aquarium. A pair of projects with the Indian mandolin wizard U. Srinivas, 1994's Rama Sreemrama and the next year's Dream, followed; in 1996, Brook reunited with Ali Khan for Night Song, trailed by work on the score for the Kevin Spacey-directed crime noir Albino Alligator.