For films it would have to be:
TRON (the original) - it was groundbreaking for the time.
TRON Legacy (obviously!)
For Anime then I was gobsmacked when a Japanese visitor left Advent Children (Final Fantasy VII spin-off) in the wastebasket - one of the male 'actors' looked lifelike - Mattel's Barbie spin-offs have got a lot to catch up to! (And no I don't have a Ken Doll!)
Computer films that impress me were: Blue (Boy dreaming about his drawn robot) on cover of PC Format a few years back, and the GNU/Linux films -
Elephant's dream: http://www.elephantsdream.org/
and Big Buck Bunny: http://www.youtube.com/watch?v=YE7Vz...eature=related
That last post by manofstrad has reminded me of a robot tramping outside Sheffield Town Hall that came on a Videogame with the last nVidia graphics I purchased for the main machine!