I loved all of these, but it's getting harder and harder to find stuff like this at Blockbuster:

American Beauty
Anything directed by Stanley Kubrick starting with Lolita.
Apostle – Robert Duvall
Barfly – Mickey Rourke.
Blood Simple – Early Coen brothers.
Boogie Nights
Clean and Sober – Michael Keaton
Cookie's Fortune
Eating Raoul
Fabulous Baker Boys – Jeff and Beau Bridges.
Grand Canyon
Gummo – but I advise caution. This isn't for everyone. Some people will hate it.
Jackie Brown
Last Seduction
Little Voice
Opposite of Sex
Runaway Train
Six Degrees of Separation
Trees Lounge – Steve Buscemi
Twenty Bucks – an ensemble cast, but it has a few famous actors in small roles