Three days before he was supposed to start shooting “Goodfellas,” filmmaker Martin Scorsese’s 1990 account of friendship, betrayal, jealousy and addiction in the New York City mob, actor Paul Sorvino was ready to quit. “Get me out,” he told his manager in a desperate phone call. “I’m going to ruin this great man’s picture, and I’m going to ruin myself.”

Mr. Sorvino had been cast as the stately but menacing mob boss Paulie Cicero, a character based on convicted mobster Paul Vario, and was having trouble with the role. Like Paulie, he was an Italian American from Brooklyn; he felt he understood the character’s speech and mannerisms, including the loving way he treated low-level gangsters like Henry Hill, the film’s protagonist (played by Ray Liotta). But he was struggling to find “that kernel of coldness and absolute hardness” that allowed Paulie to order a hit on a longtime friend or associate.

He wasn’t sure he would ever find it. Then, soon after he called his manager, he went to adjust his tie. “I looked in the mirror and literally jumped back a foot,” he later told the New York Times. “I saw a look I’d never seen, something in my eyes that alarmed me. A deadly soulless look in my eyes that scared me and was overwhelmingly threatening. And I looked to the heavens and said, ‘You’ve found it.’ ”

Mr. Sorvino, a would-be opera singer who also sculpted and wrote poetry, went on to deliver one of the most gripping performances of his career, alongside co-stars Robert De Niro, Joe Pesci, Lorraine Bracco and Liotta, who died in May at 67.

As Paulie, Mr. Sorvino never used a phone, stayed away from group conversations, instructed a philandering Henry to return to his wife and introduced millions of viewers to an unusual system for slicing garlic: using a razor blade to cut it so fine that it liquefies in the pan. “It’s a very good system,” Henry explains in a voice-over.

Mr. Sorvino was 83 when he died July 25 at a hospital in Jacksonville, Fla. His death was confirmed by his publicist, Roger Neal, who said Mr. Sorvino had health problems in recent years but did not give a specific cause.

Based on a nonfiction book by Nicholas Pileggi, “Goodfellas” received six Academy Award nominations and launched Mr. Sorvino to a new level of fame, helping him land a starring role on “Law & Order’s” early seasons as a police detective, Sgt. Phil Cerreta.

The burly, 6-foot-3 Mr. Sorvino had long played characters on both sides of the law, including Al Pacino’s overworked police supervisor in “Cruising” (1980) and the villainous, wide-mouthed gangster Lips Manlis in “Dick Tracy” (1990), directed by his friend Warren Beatty. He later played heavies in Disney’s “The Rocketeer” (1991), Sydney Pollack’s “The Firm” (1993) and two recent seasons of “Godfather of Harlem,” an Epix crime drama starring Forest Whitaker.

But those roles — elevated by the angry glower or deadly stare he would give to a co-star — were just one aspect of a wide-ranging career that included more than 170 movie and TV credits, as well as a Tony Award nomination in 1973 for starring in “That Championship Season,” a tragicomic play by Jason Miller.

“It’s almost my later goal in life to disabuse people of the notion that I’m a slow-moving, heavy-lidded thug,” Mr. Sorvino told Orlando Weekly in 2014. Interviewed by the Times in 2006, he remarked that while “everyone thinks I’m a mobster, I think of myself as a warrior-poet” — as well as a singer, a role that he further inhabited after making his New York City Opera debut later that year.

On-screen, Mr. Sorvino showed his range while playing a sentimental newspaper columnist in “Slow Dancing in the Big City” (1978), a deaf lawyer in the TV movie “Dummy” (1979), left-wing political activist Louis C. Fraina in Beatty’s “Reds” (1981), diplomat Henry Kissinger in Oliver Stone’s “Nixon” (1995) and Juliet’s father in Baz Luhrmann’s “Romeo + Juliet” (1996).

He also served as a mentor for his daughter Mira Sorvino, who followed him into show business and won an Oscar for her supporting role in “Mighty Aphrodite” (1995). “When you give me this award, you honor my father, Paul Sorvino, who has taught me everything I know about acting,” she said at the awards ceremony, as the camera found Mr. Sorvino in the audience. Lifting his arms to his face, he burst into tears.

The youngest of three sons, Paul Anthony Sorvino was born in Brooklyn on April 13, 1939, and grew up in the borough’s Bensonhurst neighborhood. His father was a garment factory foreman, and his mother was a piano teacher. From a young age, he was drawn to performing, cracking up classmates at Lafayette High School and dreaming of a career as a singer or actor.

“When I was around 3, I’d be hollering for attention and the neighbors would ask, ‘Why is Paul crying?’ Mama would tell them, ‘He’s not crying, he’s performing,’ ” Mr. Sorvino told the Times. Decades later, he still remembered the lines from his first performance, a kindergarten play: “I am Paul Oatmeal, true of heart and true of soul. Put me in your breakfast bowl.”

While listening to recordings by operatic tenors like Mario Lanza and Enrico Caruso, he started to develop his voice, learning to overcome severe asthma. He sang at bingo games, nightclubs and summer resorts in the “minestrone belt” of the Catskills, and supported himself by waiting tables, mixing cocktails at private parties and selling dictionaries door-to-door. By his early 20s he had shifted his focus to acting, winning a scholarship to study at the American Academy of Dramatic Arts, where his teachers included Sanford Meisner.

For years, he found it difficult to get work. “I had confidence in my ability, and I was angry as hell when other people didn’t recognize it,” he recalled. “Like I’d be acting my heart out at a reading only to be stopped halfway through with a ‘Thank you very much. Next?’ That kind of rejection unstrung me. I’d storm into the wings wanting to punch somebody.”

Therapy helped, he said, but for a time he simply gave up acting altogether, quitting the business to join a New York advertising agency. He rose from copy writer to vice president but was miserable. With encouragement from his wife, Lorraine Davis, he returned to show business, making his Broadway debut in 1964 in the musical comedy “Bajour.”

In 1971, Mr. Sorvino appeared in the heroin-addiction movie “The Panic in Needle Park” with Pacino and played Joseph Bologna’s father in the film comedy “Made for Each Other.” He was younger than his on-screen son, but his performance impressed Miller, the playwright, leading to his audition for “That Championship Season.”

Set at a reunion of former high school basketball players with their coach, the play won a Pulitzer Prize and ran for 700 performances on Broadway. The cast was roundly praised for its ensemble work, but Mr. Sorvino was singled out by several critics for the physicality of his performance as Phil Romano, a debauched, Porsche-driving mining executive who is having an affair with the wife of one of his old teammates.

He reprised the role for a 1982 film adaptation, which also starred Robert Mitchum and Martin Sheen, and directed a 1999 made-for-TV adaptation, this time playing the basketball team’s thunderous old coach.

Mr. Sorvino’s marriages to Davis and Vanessa Arico ended in divorce. In 2014, he married Dee Dee Benkie, a Republican political strategist whom he met in a Fox News green room when they were both appearing on the talk show “Your World With Neil Cavuto.”

After they eloped at Lincoln Center in New York, she launched an acting career, often working with her husband. “Any movie or TV show he did, she had a role,” said his publicist, Neal. The couple split their time between Los Angeles, New York City, Jacksonville, Fla., and Madison, Ind.

In addition to his wife, survivors include three children from his first marriage, Mira, Amanda and Michael Sorvino; a brother; and five grandchildren.

Explaining his childhood desire to become an actor, Mr. Sorvino told the Times in 1977, “It seemed the surest way to express my feelings, and I always had a tremendous need to do that, to have a communion with other people.”

“A lot of people become actors for the wrong reasons,” he added. “They seek the applause to make up for a lack of love. But I see acting as a sharing of love, a giving for the love of giving. The getting part of it is just the frosting on the cake.”