His early caricatures of public figures were published in satirical magazine Private Eye throughout the 1960s and 1970s. In 1979, he provided the cover illustration for Pink Floyd's The Wall and in 1982 worked on animations for the film version of the album.
In 2000, Scarfe worked on the Disney film Hercules as a conceptual character artist, and his designs were widely acclaimed.
In 1971 he met Jane Asher, with whom he had two children in 1974. They married in 1981, and had another child in 1984.