HOLY LORD. Yes to Psycho Pass (at least Season 1, haven't gotten around to 2 yet).

Pardon me for jacking in at random spots, still not sure the best places to pop in at this point.

And from the little I've scraped so far, so long as you're looking toward Samurai Champloo, I'd recommend Cowboy Bebop as the one to go to as well. It's definitely in similar vein so far as classics, and, in fact, made by the same person as Champloo.

This is in a different direction of sorts, although if/when ever you find yourself in Manga for any odd reason, I'd recommend Gantz with the weight of everything I am. It's a phenomenal epic of a Manga beautifully illustrating the hero's journey in its own way; furthermore, I Am a Hero.

But I digress.

I'm more so into the short 12-24 episode anime series. They can take time to go into where movies can't in some ways. Although, Rurouni Kenshin: Trust and Betrayal is in the style of 3 short movies that earned its merit in its own rite (right?).

If you'd like me to expand on any of these with theme/plot or the like, feel free to post and I'll expound all I can without spoilers.