“As far back as I can remember, I always wanted to be a gangster.” Those words, delivered with lingering fascination by the actor Ray Liotta, who has died unexpectedly aged 67, ushered audiences into Martin Scorsese’s Goodfellas (1990), one of the most dynamic pictures made about the criminal life and its enticements.

Liotta, playing the real mobster-turned-informant Henry Hill, has just been seen taking part in the fatal knifing of a mob rival when the camera zooms on to his face, bathed in the infernal red glow of a car’s brake-lights. Seductive and terrifying, he exudes a charred handsomeness and a chilling self-belief. Though Goodfellas was only his fourth major screen role, Liotta was seen (and heard, in a matter-of-fact voiceover) for much of the movie’s two-and-a-half-hour running time.

He held his own in the company of experienced co-stars such as Robert De Niro and Joe Pesci, who played fellow hoods. His fizzy, feisty rapport with Lorraine Bracco, as Henry’s wife, Karen, brought valuable warmth to the intense, sometimes harrowing, material.

Take any of the movie’s most memorable scenes and Liotta is at the heart of them: the technically complex single-take Steadicam shot, which doubles as a portrait of Henry’s rise in miniature as it follows him and Karen from the streets into the back entrance of the Copacabana nightclub, through its corridors and kitchens, and ends up at their VIP table for that evening’s show; the mortifying moment when Henry makes the mistake of referring to the volatile Tommy (Pesci) as “a funny guy”, unleashing in the process an intimidating tirade; and the virtuoso sequence late in the film in which Henry, frazzled on cocaine, plagued by paranoia and pursued by the Feds, finally runs out of luck.

He is last seen standing on a doorstep in his dressing gown, staring into the camera as he contemplates life in the witness protection programme. “I’m an average nobody,” he complains in the voiceover. “I get to live the rest of my life like a schnook.”

Goodfellas made Liotta a star but he had already given an equally magnetic performance in Something Wild (1986), his first lead role. He was 30 when he was cast as Ray Sinclair, a thug who terrorises his free-spirited ex-wife, Audrey (Melanie Griffith), after being released from prison.

Jonathan Demme’s masterful comedy-thriller is a movie of two halves, its audacious shift from high-jinks to horror resting largely on Liotta’s shoulders. When he looms into view on the dancefloor at a high-school reunion, spooking Audrey and her date (Jeff Daniels), it is one of the most spine-tingling moments in modern cinema, as well as a warning to audiences who had been blithely enjoying the previous hour that the fun and games were now over. His mercurial quality, his gift for stillness, his arctic blue eyes – all these were assets in portraying a brute who nevertheless remains compellingly human.

It helped no end that Liotta was an unknown quantity, at least to those who had not seen him on television during his three years in the soap opera Another World (1978-81), where he played “the nicest guy in the world”.

In later years, he often insisted that he had been unfairly pigeonholed as a villain or a gangster. It was for that reason that he turned down a part in the third series of The Sopranos, though he did appear in the show’s movie prequel, The Many Saints of Newark (2021), as well as playing the mobster Roy DeMeo in The Iceman (2012). Chagrined that “bad guys just seem to stand out”, Liotta protested that he wasn’t “a criminal or a tough guy or a gang member. My life does not revolve around intensity … I like playing the nicer guy in movies. I can relate to them better.”

He played the twin brother of a man (Tom Hulce) with learning difficulties in Dominick and Eugene (1988), but his most beloved “nice guy” role was in Field of Dreams (1989), a sentimental fantasy about a farmer (Kevin Costner) who builds a baseball field that is then frequented by the ghosts of long-dead players.

Among them is “Shoeless” Joe Jackson, who is played by Liotta with an unusual twinkling softness, as well as a steely undertone that keeps his performance focused even as the film makes its assault on the tear ducts.

He could be disarmingly vulnerable in harsher contexts, too. The most shocking scene in the crime movie Killing Them Softly (2012) occurs when Liotta, as a luckless card sharp, bursts into tears while being beaten up, a sight simultaneously moving, upsetting and unshakably strange.

He was born in Newark, New Jersey, where he was adopted at six months old and raised by Mary, a township clerk, and Alfred Liotta, who owned an auto parts store. Ray had grown up believing he was of Italian heritage, but on meeting his birth mother in his 40s, discovered his origins were in fact Scottish. He was educated at Union high school, in his home state, and at the University of Miami, where he studied drama.

He enjoyed acting on stage there, and later moved to New York, where he was cast in commercials and television series before auditioning successfully for Something Wild.

Though he never became a superstar – he expressed regret that he had declined an offer to meet Tim Burton, who wanted him to play Batman in his 1989 film – he worked consistently. He was a cop menacing Kurt Russell and Madeleine Stowe in Unlawful Entry (1992); in fact, violent or corrupt cops would later became something of a speciality of his in the likes of Narc (2002) and The Place Beyond the Pines (2012).

In a gentler register, he played a widower who hires a nanny (Whoopi Goldberg) for his daughter in Corrina, Corrina (1994), then starred in the thriller Unforgettable (1996), the airborne action movie Turbulence and the more thoughtful crime drama Cop Land (both 1997), which co-starred De Niro, Sylvester Stallone and Harvey Keitel.

When he played Frank Sinatra in the TV movie The Rat Pack (1998), he received a fake horse’s head in the mail (a Godfather reference) from the singer’s daughters, who were aggrieved that he had turned down their offer to play their father in a competing project.

He was an unsavoury justice department agent in Hannibal (2001), where he had the dubious privilege of being at the centre of its grisliest scene: sitting upright but partially anaesthetised at the dinner table, he is fed parts of his own brain – sautéed, no less – by the cannibalistic killer played by Anthony Hopkins. He was also Johnny Depp’s father in the drugs-and-crime drama Blow (2001), which owed a considerable stylistic debt to Goodfellas.

Later films included the thrillers Identity (2003) and Guy Ritchie’s Revolver (2005), as well as the biker comedy Wild Hogs, with John Travolta. Liotta had a ball playing himself in Jerry Seinfeld’s animated Bee Movie (2007), where he is the purveyor of his own brand of honey, and appeared alongside Kermit the Frog and co in Muppets from Space (1999) and Muppets Most Wanted (2014). In 2005 he won an Emmy for a guest appearance on the TV drama ER.

Forthcoming productions include the Apple TV drama Black Bird, in July, in which Liotta plays the police-officer father of a drug-dealing son, and what he termed the “nutty” movie Cocaine Bear, due for release next February. His standout performance of recent years was as a remorseless divorce lawyer in the Oscar-winning Marriage Story (2019). Like all his best work, it was authentic, direct and unfussy. “I don’t do things to find out about myself,” he said. “I just like playing pretend.”

Liotta was shooting a film, Dangerous Waters, in the Dominican Republic when he was found dead in his hotel room.

His fiancee, Jacy Nittolo, survives him, as does a daughter, Karsen, from his marriage to Michelle Grace, which ended in divorce.

• Raymond Allen Liotta, actor, born 18 December 1954; died 26 May 2022