He went on to play many supporting roles in films such as Jungle Fever (1991), Bad Boys (1995), The Basketball Diaries (1995), Shark Tale (2004), The Lovely Bones (2009), and One Night in Miami (2020).

[6][7] At age 11, Imperioli and his family moved to Brewster, New York, and in high school he began watching Broadway plays.

[3] After graduating from Brewster High School in 1983,[8] Imperioli planned on studying pre-med at the State University of New York at Albany.

At age 17, Imperioli then moved to Manhattan's East Village, where he enrolled at Lee Strasberg Theatre and Film Institute to study acting.

[3][4] In the early 1990s, Imperioli performed as lead vocalist of the New Jersey-based jangle pop band Wild Carnation, departing to focus on his acting career prior to the release of their debut recordings in 1993.

[10] In addition to his role on The Sopranos, Imperioli has appeared in a number of films, including Goodfellas, Jungle Fever, Bad Boys, Malcolm X, The Basketball Diaries, Clockers, Dead Presidents, Girl 6, My Baby's Daddy, Lean on Me, I Shot Andy Warhol, Last Man Standing, Shark Tale, High Roller: The Stu Ungar Story, and Summer of Sam, which he also co-wrote and co-produced.

Imperioli won the Tournament of Stars competition on the cooking show Chopped in 2014, sending $50,000 to his designated charity the Pureland Project, an organization which builds and maintains schools in rural Tibet.

[15] On March 13, 2019, Imperioli was cast in the lead role of Rick Sellitto in the NBC drama series Lincoln Rhyme: Hunt for the Bone Collector.

[25] Imperioli portrayed Andrew Cuomo in the Showtime limited series Escape at Dannemora (2018), Angelo Dundee in the Regina King directed One Night in Miami (2020), and served as narrator in the 2021 Sopranos prequel film, The Many Saints of Newark.

In 2023 it was announced that Imperioli would make his Broadway debut in the 2024 Sam Gold-directed adaptation of the Henrik Ibsen play An Enemy of the People, acting alongside Jeremy Strong and Victoria Pedretti at the Circle in the Square Theatre.