It's pretty hard to think of a series that would look good on a large screen.
I never tried it but something eccentric like Afro Samurai would create an interesting effect imo
If you pay more attention to artistic merits, I would recommend KyoAni's line of animation for good background arts and bright overall scheme if you are into their focus genre.
I guess I can recommend Makoto Shinkai's 5 Centimeters Per Second if you want to venture into the movie genre. I would have this movie playing all the time on my large screen if my sister didn't have a nervous breakdown every time she heard the song "One more time, One more chance" (and I go off the topic)
