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The last Williams movie released during his lifetime was The Angriest Man in Brooklyn, a film addressing the value of life. In it, Williams played Henry Altmann, a terminally ill man who reassesses his life and works to redeem himself.

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In the 2002 film Insomnia, Williams portrayed a writer/killer on the run from a sleep-deprived Los Angeles policeman (played by Al Pacino) in rural Alaska.

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Other roles Williams had in acclaimed dramatic films include Moscow on the Hudson (1984), Awakenings (1990) and What Dreams May Come(1998).

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In 1991, he played an adult Peter Pan in the movie Hook, although he had said that he would have to lose twenty-five pounds.

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two previous Academy Award nominations (for playing an English teacher in Dead Poets Society (1989), and for playing a troubled homeless man in The Fisher King (1991)

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Williams was allowed to play the role without a script, improvising most of his lines. Over the microphone, he created voice impressions of people, including Walter Cronkite, Gomer Pyle, Elvis Presley, Mr. Ed, and Richard Nixon.

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His first major break came from his starring role in director Barry Levinson's Good Morning, Vietnam (1987), which earned Williams a nomination for the Academy Award for Best Actor.

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His first major performance is as the title character in Popeye(1980). There, Williams showcased the acting skills previously demonstrated in his television work; and the film's commercial disappointment was not blamed upon his role.