The cause was congestive heart failure, said his son Jeff.

A self-described “tough kid from the streets,” Mr. Persoff grew up in Brooklyn during the Depression and was working as a subway electrician in the late 1930s when — having shaved his head for relief from the summer heat — he caught the attention of an off-Broadway producer looking to add “local color” to his production.

Mr. Persoff agreed to appear onstage and found the experience thrilling, an escape from his mundane existence. In 1948, after Army service in World War II, he became an early member of the Actors Studio, a workshop in New York founded by director Elia Kazan and other prominent figures in theater.

From that elite training ground, Mr. Persoff, already approaching 30, launched a prolific career in the early days of TV. With his stocky build, unnerving gaze, five o’clock shadow and tightly wound energy, Mr. Persoff specialized in portraying gangland figures, Wild West desperados, bellicose generalissimos and Cold War heavies.

Trading his grimace for a warm smile on his broad, expressive face, he also played men of the cloth and workaday laborers in crisis. Like his Actors Studio classmate Eli Wallach, who was also Jewish, he was in constant demand to play ethnic characters including Egyptians, Moroccans, Greeks, Italians and Russians.

His TV career was so prodigious in the 1950s and ’60s that he frequently raced between sets for episodes of such shows as “Rawhide,” “Route 66” and “The United States Steel Hour” — switching wardrobes, hairpieces, prosthetic features, mannerisms and accents at a frantic pace. Although a jovial and peaceable presence off-screen, he was admired for his ability to tap into reservoirs of anger, especially when playing characters with a strong streak of rebelliousness against authority.

“If a character is within my range, then I can find him within myself,” he told the Los Angeles Times in 1958. “This character is me under different circumstances. Logic is always on the side of a character. It’s up to me to rationalize the validity of his action.”

In two of his most acclaimed roles of the period — both in 1959 on the dramatic anthology show “Playhouse 90” — he played Italian dictator Benito Mussolini in a teleplay called “The Killers of Mussolini” and the melancholy Spanish guerrilla Pablo in an adaptation of Ernest Hemingway’s “For Whom the Bell Tolls.”

“Bearded, boorish and beat, he swiped the show out from everyone else,” United Press International TV critic William Ewald wrote of Mr. Persoff’s portrayal of Pablo in a cast that included Jason Robards, Maureen Stapleton, Maria Schell and Wallach. “He caught magnificently the minglement of barbarity and civilization, butcher and shattered hero.”

On “The Twilight Zone,” Mr. Persoff portrayed the skipper of a German U-boat that attacks a British freighter in World War II without warning. The sub sinks the helpless ship, the sub’s crew machine-guns the survivors and the skipper is doomed to relive the episode, from the other side, for eternity.

He became a regular guest star on such disparate shows as “Gilligan’s Island,” playing an exiled tinhorn autocrat named Pancho Hernando Gonzalez Enriques Rodriguez, and “The Untouchables,” as an Al Capone mob associate named Jake “Greasy Thumb” Guzik.

He made an indelible impression in filmmaker Billy Wilder’s celebrated comic romp “Some Like it Hot” (1959). As the crime boss Little Bonaparte — standing under a banner inscribed with “Friends of Italian Opera” — he proudly announces to an assembly of crime syndicate members: “In duh lass fissel year, we made one hundred an’ twelve million dollars before taxes — only we ain’t payin’ no taxes!” He wears a hearing aid that he turns off when a spray of bullets rubs out his rivals.

His later film roles included the high priest Shemiah in the all-star biblical epic “The Greatest Story Ever Told” (1965), a Jewish refugee in flight from the Nazis in “Voyage of the Damned” (1976), Barbra Streisand’s scholarly and caring father in the movie musical “Yentl” (1983), and the scientist behind a eugenics experiment in the comedy “Twins” (1988), starring Danny DeVito and Arnold Schwarzenegger as the unlikeliest of siblings. He also was the voice of the animated mouse patriarch Papa Mousekewitz in “An American Tail” (1986) and its film sequels.

After suffering a stroke at 70, Mr. Persoff slowed down his acting career and took up watercolors — approaching the new medium with the same intensity he channeled into his acting. He worked night and day, he said, and amassed a portfolio of more than 250 paintings.

He likened his new art form to the old one.

“When I got a role, I set my sights on being able to get under the skin of the character,” he told interviewer Nick Thomas. “It’s the same with painting. When you sit in front of a blank canvas, there is a feeling of ‘I can’t do it’ for many painters. But because of my acting experience, I always felt that I could do it, and I did.”

Mr. Persoff was born in Jerusalem — soon to become part of the British mandate of Palestine — on Aug. 2, 1919. His father, a coppersmith and jeweler, settled with his family in Brooklyn a decade later. Mr. Persoff, known as Nicky in the United States, described his family as impoverished but tightknit.

He attended the Hebrew Technical Institute, a vocational high school in Manhattan, before doing signal maintenance for the city subway system. After working with amateur theater troupes, he auditioned for the New Theatre League acting school, where he was told that he could attend for free in exchange for fixing any broken lights.

While studying at the Actors Studio, alongside Marlon Brando and Montgomery Clift, he had supporting roles on Broadway before Kazan tapped him to play a mobbed-up cabbie in the movie drama “On the Waterfront” (1954). As the sinister cabdriver, he witnesses the famous “I coulda been a contender” speech by ex-boxer Terry Malloy (played by Brando) and then takes Malloy’s corrupt older brother, Charley (played by Rod Steiger), for his final ride.

“There were Brando and Steiger in the back section of a sawed-off car,” Mr. Persoff told Thomas. “I sat on a milk box with Brando and Steiger behind me. When it was time for my close-up, Kazan whispered in my ear to imagine that ‘the guy behind you killed your mother.’ When I saw the film, I was surprised to see how effective the close-up turned out.”

Mr. Persoff played the right-hand man to Steiger’s corrupt boxing promoter in “The Harder They Fall” (1956) and a jittery sergeant blown up by a land mine in the Korean War film “Men in War” (1957), among other small but standout movie roles.

His career continued at a relentless pace through the 1980s, after which he made occasional appearances on “Law & Order,” “Chicago Hope” and other series. His final role, in 2003, was as a rabbi in the HBO production of “Angels in America,” based on Tony Kushner’s play about the AIDS epidemic. He also toured the country for years in a one-man show, “Sholem Aleichem,” telling stories by the Yiddish humorist and playing some of his characters, and he wrote a memoir, “The Many Faces of Nehemiah,” published in 2021.

His wife, Thia Persov, a distant cousin, died in 2021 after 69 years of marriage. In addition to his son Jeff, survivors include three other children, Dan, Perry and Dahlia; and five grandchildren.

Reflecting on his prolific career, he told author Darryl Lyman for the book “Great Jews in the Performing Arts” that he saw his work ethic as a rebuke to Adolf Hitler and the antisemitism that persisted long after the Nazi dictator’s defeat.

“I suspect that one of the most powerful forces shaping my life when I was growing up in the U.S.A. was that German with the small mustache who questioned the right of my people — and therefore me — to live,” he said. “I was then determined to develop whatever talent I had to prove worthy of the gift of life.”