Based on "emotional value", here's my Top 9:
1. Scryed - Best series, ever! Has yet to be topped in my book. The story is basically about "alter" users, people with supernatural powers. Think X-Men, with much more tension - the character design is simply amazing, you care so much for everyone.
2. Naruto - a ninja series that is still in progress. Grabs you tight and won't let go. Each episode has more or less mean cliffhangers making you want more and more.
3. Angelic Layer - Cute series that distantly resembles Pokemon, but with more heart and spirit. Has a grand and unforgettable finale. Just adorable.
4. 3x3 Eyes - Fantasy, Magic, Mystery. Features one of the best main characters in any anime (Pai) and has a very good story.
5. Rurouni Kenshin - Looong and kind of sad story about a lone wanderer, a legendary manslayer. Recommended.
6. X-TV - Dark and mystic. Dreamlike even.
7. Read or Die - Three part OAV about people with very interesting supernatural powers.
8. Neon Genesis Evangelion - I guess everyone is familiar with this...
9. Infinite Ryvius - Space series, was made before Scryed by the same team. Similarly marvelous character design.