Peter O’Toole, an Irish bookmaker’s son with a hell-raising streak whose performance in the 1962 epic film “Lawrence of Arabia” earned him overnight fame and established him as one of his generation’s most charismatic actors, died on Saturday in London. He was 81.

His daughter Kate O’Toole said in a statement that he had been ill for some time.

Blond, blue-eyed and well over six feet tall, Mr. O’Toole had the dashing good looks and high spirits befitting a leading man — and he did not disappoint in “Lawrence,” David Lean’s wide-screen, almost-four-hour homage to T. E. Lawrence, the daring British soldier and adventurer who led an Arab rebellion against the Turks in the Middle East in World War I.

The performance brought Mr. O’Toole the first of eight Academy Award nominations, a flood of film offers and a string of artistic successes in the ’60s and early ’70s. In the theater — he was a classically trained actor — he played an anguished, angular tramp in Beckett’s “Waiting for Godot” and a memorably battered title character in Chekhov’s “Uncle Vanya.” In film, he twice played a robust King Henry II: first opposite Richard Burton in “Becket” (1964), then with Katharine Hepburn as his queen in “The Lion in Winter” (1968). Both earned Oscar nominations for best actor, as did his repressed, decaying schoolmaster in “Goodbye, Mr. Chips” in 1970 and the crazed 14th Earl of Gurney in “The Ruling Class” in 1973.

Less successful was his Don Quixote in “Man of La Mancha,” Arthur Hiller’s 1972 adaptation of the Broadway musical, but it emphasized that his specialty was increasingly becoming the outsider or misfit: dreamy, romantic, turbulent, damaged, or even mad, but usually larger than life.

Mr. O’Toole threw himself wholeheartedly into what he called “bravura acting,” courting and sometimes deserving the accusation that he became over-theatrical, mannered, even hammy. His lanky, loose-jointed build; his eyes; his long, lantern-jawed face; his oddly languorous sexual charm; and the eccentric loops and whoops of his voice tended to reinforce the impression of power and extravagance.

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