Mushishi is a really gorgeous show. It was really amazing to see a tv show animated in 1s and 2s, in the second episode when the little girl open her eyes I was like "no way" and there's a lot of OMG moments in this show. Wolf's rain is amazing too, the wolves were really well done, the animation was good for the most part.
Dennou Coil had very rich animation, the mannerisms in the kids, the gorgeous layouts, the charming music, very ghibli like. I never expected to see a show that beautiful again until Xam'd Lost memories, which was another really well produced tv show, the explosion in the beginning of the second episode is just WOW, you don't see that kind of stuff very often in TV.
In movies I think Ghost in the Shell 2: Innocence, Jin Roh, and Blood: The Last Vampire are still my favourites. The characters designs are realistic and that's the style I like the most.The shadows are so impressive in GITS 2 and they did something similar with the shadows in Otogi Zoshi but the animation wasn't that good.
The art looks amazing in the op
http://www.youtube.com/watch?v=2MDK8WHQawE