Scott was in much demand for guest shots on TV shows, appearing in episodes of Ben Casey and Naked City. In 1962, Scott appeared as school teacher Arthur Lilly on NBC's The Virginian, in the episode "The Brazen Bell", in which he recites Oscar Wilde's poem "The Ballad of Reading Gaol". That same year, he appeared in NBC's medical drama The Eleventh Hour, in the episode "I Don't Belong in a White-Painted House". He appeared opposite Laurence Olivier and Julie Harris in Graham Greene's The Power and the Glory in a 1961 television production and also performed in The Merchant of Venice (1962) off-Broadway.
Scott portrayed George S. Patton in the film Patton (1970) and researched extensively for the role, studying films of the general and talking to those who knew him. Scott refused the Oscar nomination for Patton, just as he had done for his nomination in 1962 for The Hustler, but won the award anyway.