Alright, time to kick this category off.
I say that the best anime has got to be Wolf's Rein.
The storyline is great, you can relate to the characters...well....some of them anyway, and it's short (only like 30-something episodes), so it doesn't drag on forever with the same thing in every episode. For example, in Inuyasha, I think Kagome told him to sit like 1000 times, Miroku groped Sango and got smacked every other episode, and it just got annoying after a while. I like Wolf's Rein, because every episode is different, and every episode advances the story.
Also, the whole human-looking wolf thing was kinda cool, in my opinion.