My favorite character is William Holden's "Pike Bishop," the leader of the Bunch.
There are so many great moments in this classic film it's hard to pick one as a favorite, but if I had to, I'd have to say the ending, when Edmond O'Brien's "Freddy Sykes" asks Robert Ryan's "Deke Thornton" "you wanna come along? It ain't like it used to be, but it'll do" -- and then O'Brien's cackling, contagious laughter, triggering Ryan's own, accompanying laughter, leading to the final images of the Bunch, laughing uproariously, lustily, and ironically.