I always enjoy proper minor villain roles, the guys who leave an indelible mark despite maybe only appearing briefly and frequently being dispatched at the end of their scene or two. James Gandolfini in True Romance Stephen McHattie as a perfectly hateful killer who sets the story’s events in motion in A History of Violence Said Taghmaoui in Three Kings (more a gray area role than outright villain) Timothy Carey in The Killing more major roles but Lance Henriksen in Hard Target*, Near Dark, Johnny Handsome, and Stone Cold * special shout out to Arnold Vosloo in that one too
Travolta's played quite a few bad guys. I liked him in Swordfish, Face Off, and The Taking of Pelham 123.
Six pages in and no mention of two of the great heavies ...William Smith (RIP) and Al Lettieri Sollozzo in The Godfather fame
Off the top of my head: Lee Marvin Claude Akins John Russell Dan Duryea Robert J. Wilke Warren Oates John McIntyre
Mark Hamill as The Joker in the Animated DC Universe. For me, he is more memorable for that role than that of Luke Skywalker. See the following video for the various actors who have played and voiced The Joker and compare:
That made me think of Reggie Nalder .. .. who played a lot of baddies in his time and the scariest TV vampire.. (Fun fact - according to IMDb he was onscreen for less than 90 seconds during the 3 hour mini series)