Finch's film roles increased in size and prestige through the early 1950s. For Walt Disney he played the Sheriff of Nottingham in The Story of Robin Hood and His Merrie Men (1952). He was given two good roles in films from Alexander Korda: as Richard D'Oyly Carte in The Story of Gilbert and Sullivan (1953), and as a priest in The Heart of the Matter (1953), from the Graham Greene novel.
He was soon cast in his first British movie, playing a murderous actor in Train of Events (1949). Critic C. A. Lejeune praised his work in the London Observer commenting that he "adds good cheekbones to a quick intelligence and is likely to become a cult, I fear." The Scotsman said "he should be regarded as one of the most hopeful recruits to the British screen."
He did radio acting work with Hugh Denison's BSA Players (for Broadcasting Service Association, later to become Macquarie Players). He came to the attention of Australian Broadcasting Commission radio drama producer Lawrence H. Cecil, who was to act as his coach and mentor throughout 1939 and 1940. He was "Chris" in the Children's Session and the first Muddle-Headed Wombat.
Finch's next three films saw him support notable female stars: Sophia Loren in Judith (1966), Melina Mercouri in 10:30 P.M. Summer (1966) and Julie Christie in Far from the Madding Crowd (1967). He was reunited with Aldrich for The Legend of Lylah Clare (1968). The Red Tent (1970) was an expensive international adventure film, with Finch as Umberto Nobile.
In 1980, American author Elaine Dundy published a biography of Finch titled Finch, Bloody Finch: A Biography of Peter Finch. That year, his second wife, Yolande Finch, also published a posthumous account of their life together, Finchy: My Life with Peter Finch. Another biography had previously been published by his friend and colleague Trader Faulkner, in 1979.
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During this time, Finch continued to appear on stage in various productions while under contract to Olivier. Finch's closeness to the Olivier family led to an affair with Olivier's beautiful but increasingly unstable wife, Vivien Leigh, which began in 1948, and continued on and off for several years, ultimately falling apart due to her deteriorating mental condition.