Pastore has made a career of playing the parts of Italian-American mobsters. He began with small parts in 1990's GoodFellas and 1993's Carlito's Way. In GoodFellas, he is briefly seen rolling a coat rack through the kitchen of The Copacabana and is credited as Vincent Pastore playing Man with Coat Rack. In Carlito's Way, he is one of the friends of the Italian man that dances with Gail, whom Kleinfeld insults. He is listed in the credits as Vinny Pastore playing Copa Wiseguy.
Pastore got a bigger role in the comedy/crime film The Jerky Boys (1995) as Tony Scarboni, one of the three gangsters and Lazarro (Alan Arkin)'s clients. In the 1996 HBO television movie Gotti, Pastore played the character of Angelo Ruggiero, alongside fellow Sopranos cast members Tony Sirico and Dominic Chianese.
In 1999, Pastore got his biggest role to date in The Sopranos, where he played the character Salvatore Big P***y Bonpensiero. His character was murdered in the finale of season 2, but Pastore would make a few more appearances over the next few years in dream and flashback sequences.
Following The Sopranos, he appeared in Mickey Blue Eyes, Two Family House (with Sopranos cast mates Michael Rispoli, Kathrine Narducci, Matt Servitto, Michele Santopietro, Louis Guss, Rosemary De Angelis, and Sharon Angela), Under Hellgate Bridge, Riding in Cars with Boys. Deuces Wild, Made, Mafia!, The Hurricane, Serving Sara, Carlito's Way with Sean Penn, American Cousins, A Tale of Two Pizzas, This Thing of Ours, Shark Tale , Johnny Slade's Greatest Hits, and Guy Ritchie's Revolver. He served as Associate Producer of the film, Doughboys. Television credits include Grounded for Life (2002), character Vinnie Fellachio in Son of a Beach (2002), Law & Order (various roles from 1992 1996), soap opera, One Life to Live, hosted Repo-Men/Stealing for a Living, Ed, Queens Supreme, Vegas, and Everybody Hates Chris.
In 2007, he starred in the independent feature film P.J., co-starring with Sopranos co-star John Heard and Robert Picardo.
In 2008, Pastore entered Daytime, joining the cast of General Hospital as Maximus Giambetti, father of two characters on the show. He once again plays a mobster. He had a role in 2008's College Road Trip, with Martin Lawrence and Raven-Symon, as well as in Our Last Days As Children. Pastore also starred in the film Dough Boys, released in 2008.
In 2009, Pastore will star in Pavaline Studio's debut film short Alienated.