I see 'Psycho' was mentioned above by walkerboh (great username, btw), that's a good one, and Alfred Hitchcock has so many more good movies to choose from, you could put his films in your library and they would about fill it up by themselves.
Rope
North By Northwest
Vertigo
Rear Window
The Man Who Knew Too Much
The Birds
Lifeboat
Notorious
Those were just a few.
Here's a boxed set of some of his films:
The Alfred Hitchcock Signature Collection