For me he will always be the mob limo driver in John Favreau's first feature (as director), Made (2001). It's silly and yet such a gem of a little union-made film shot entirely on location in L.A., Manhattan, Queens, and Brooklyn.
Widow's Bay DSARIP Vincent Pastore, Pussy is obviously the big one but I will also always remember him for the only truly great joke in Shark Tale, where he says over the phone “nod your head if you understand. Now tell me whether you nodded your head.”