No. 4 Jimmy Conway (Goodfellas, 1990)
Yet another acclaimed collaboration with Scorsese, this was De Niro’s return to gangster-dom (he hadn’t done a mobster film since Sergio Leone’s epic Once Upon A Time In America in 1984.) He won raves for his portrayal of tough guy James “Jimmy” Conway, mentor and confidant to up-and-coming gangster Henry Hill (Ray Liotta.)