Only pick one. I've gone back and forth over the years, I've always thought it came to either Vertigo or Psycho. I used to say Vertigo, but now I've taken the popular opinion pick - I would say Psycho was his best movie. Followed by Vertigo and North by Northwest.
Psycho is just such an incredible and ground-breaking film, it's hard to argue with it as #1. I'd say #2 is a toss-up between Vertigo and The Birds.