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Harry Dean Stanton, the gaunt, hollow-eyed, scene-stealing character actor who broke out of obscurity in his late 50s in two starring movie roles and capped his career with an acclaimed characterization as a corrupt polygamist on the HBO series “Big Love,” died on Friday in Los Angeles. He was 91.

His death, at Cedars-Sinai Medical Center, was confirmed by his agent, John S. Kelly.

Mr. Stanton spent two decades typecast in Hollywood as cowboys and villains before his unusual talents began to attract notice on the strength of his performances in the movies “Straight Time” (1978); “Alien,” “Wise Blood” and “The Rose” (all 1979); and “Escape From New York” (1981).

In those roles — as a former criminal bored in the law-abiding world, a 22nd-century space traveler, a street preacher pretending to be blind, a devastatingly cruel country-music star and a crazed demolitions expert — his look and his down-home voice were the same, but his characters were distinct and memorable.

Vincent Canby wrote in The New York Times in 1978 that Mr. Stanton’s “mysterious gift” was “to be able to make everything he does seem immediately authentic.” The critic Roger Ebert once wrote that Mr. Stanton was one of two character actors (the other was M. Emmet Walsh) whose presence in a movie guaranteed that it could not be “altogether bad.”

But he remained largely unknown to the general public until 1984, when the seemingly impossible, or at least the unexpected, happened: Mr. Stanton, the quintessential supporting player, became a leading man.

That year he starred as a wandering amnesiac reunited with his family in Wim Wenders’s “Paris, Texas,” which won the Palme d’Or at the Cannes Film Festival, and as a fast-talking automobile thief training Emilio Estevez in the ways of his world in Alex Cox’s cult comedy “Repo Man.”

If there was any remaining doubt about his newly attained star status, it was eliminated in 1986 when he was invited to host “Saturday Night Live.”

Mr. Stanton was never anonymous again, although he continued to make his contributions almost entirely in supporting roles. He played Molly Ringwald’s underemployed father in the teenage romance “Pretty in Pink” (1986), the apostle Paul in Martin Scorsese’s “The Last Temptation of Christ” (1988), a private eye in David Lynch’s “Wild at Heart” (1990), a judge in Terry Gilliam’s “Fear and Loathing in Las Vegas” (1998), the hero’s ailing brother in Mr. Lynch’s “The Straight Story” (1999), a veteran inmate cheerfully testing the electrocution equipment in “The Green Mile” (1999) and Charlie Sheen’s father in “The Big Bounce” (2004).

Mr. Stanton was cast in one of his best-known roles when he was almost 80: that of Roman Grant, a self-proclaimed prophet with 14 wives, on “Big Love,” HBO’s acclaimed series about the everyday lives of polygamists. After his character was killed in the Season 3 finale in 2009, he joked that the show had generated more response than anything else he had done, “except for a couple hundred other movies.”

Mr. Stanton had an impressive singing voice and toured with a male chorus early in his career. He first sang on screen in “Cool Hand Luke” (1967), doing three numbers, including the hymn “Just a Closer Walk With Thee.” He later formed the Harry Dean Stanton Band, which played rock, blues, jazz and Tex-Mex numbers in Los Angeles nightclubs and on tour.

In 2014 he released an album, “Harry Dean Stanton: Partly Fiction,” consisting of songs he sang on the soundtrack of a documentary about him by the same name.

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Mr. Stanton remained busy to the end. He had small roles in the 2012 movies “The Avengers” and “Seven Psychopaths” and was in episodes of the HBO series “Getting On” in 2013 and 2014. This year, he appeared in a few episodes of “Twin Peaks: The Return” and starred in the feature film “Lucky,” scheduled for release this month. He plays a hard-bitten 90-year-old atheist in the movie, which also stars Mr. Lynch.

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If there was any remaining doubt about his newly attained star status, it was eliminated in 1986 when he was invited to host “Saturday Night Live.