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After working as a camera operator on films for Michael Powell and Emeric Pressburger, Unsworth made his debut as cinematographer on the documentary feature The People's Land in 1941.
His film work brought him an impressive array of awards, including five British Society of Cinematographers awards, three BAFTAS and two Academy Awards. Unsworth was especially in demand as cinematographer in two very different genres, period pieces and science fiction. Among the highlights of his career, he collaborated with Stanley Kubrick on the visually innovative 2001: A Space Odyssey and Bob Fosse's dark musical exploration of the end of Weimar Germany, Cabaret. On a lighter film, such as Murder on the Orient Express his lighting and use of diffusion capture the danger and romance of the train while graceful integration of camera movement and optical effects contributes to the realism of the set while controlling the claustrophobia of the setting.
Unsworth's work reached its widest audience with one of his final projects, Richard Donner's Superman in 1978. Here he was responsible for integrating the work of a who's-who of cinematographers and visual effects designers, (including Zoran Perisic, an animation stand crew member from 2001, who extended Kubrick's front projection technique for Superman) with the plausibility and sense of grandeur befitting a (mostly) reverent take on a superhero. The style he developed alongside director Donner was essentially that of a science-fiction period film; the glamorous, often highly diffused cinematography observed a panoply of images of Americana, suggesting an epic timeframe for the film's scenes, a mythic America somewhere between the 1930s of the original comics and the 1970s. The style of the sequences that did not involve extensive science-fiction elements had to match scenes displaying Superman's extraordinary powers.
Unsworth was not named in the Special Achievement in Visual Effects Academy Award the film received, but instead as Director of Photography, and without a separate credit for special effects work he would not have been eligible. Donner expressed great disgust that the Academy of Motion Picture Arts and Sciences did not recognize Unsworth with an Academy Award nomination for Best Achievement in Cinematography in 1979.
Unsworth died of a heart attack in France at the age of 64 while filming Roman Polanski's Tess in 1978. He had won an Academy Award for Cabaret in 1972, and he was posthumously nominated and awarded his second Oscar for Tess, along with Ghislain Cloquet. Cloquet alone was nominated, again successfully, for the César Award for Cinematography.
He was also admired for his charming manner at work. For instance, Margot Kidder was flattered when he arranged lighting for her shots and insisted on concentration by saying, "Quiet, I'm lighting the Lady." His wife, Maggie Unsworth, worked in the British film industry, often as a script/continuity supervisor.