Cowboy bebop, Samurai Champloo, and Deathnote have my vote, with Trigun trailing behind a bit (good story, great characters, less than stellar writing) but I am going to watch Code Geass now, like right now. I had been on the fence for a while, but this topic has pushed me over.
To Jomiba, totally entitled to your opinion, even if it's the wrong opinion ;) But Cowboy Bebop is such a fantastic anime because it is a master of subtlety. It does have high style, and great music going for it, but alot of animes have that. The reason it gets such accolades though is that it avoids what so many other animes jump into, such as lengthy awkward and unnecessary exposition, and beating you over the head with over the top emotions and sentimentality.
When spike goes to see the woman at the bar before confronting Vicious in episode 5 or 6 (can't remember), he looks at a picture of himself, the woman and another man sitting on her bar. Most animes would have a ten minute flash back and a long diatribe explaining his history with them, what happened the the husband, and some emotional scenes of spike feeling terrible and trying not to cry. But Cowboy bebop gives you the sense of what you need to know about their relationship and their past with just a glance at the picture and a few sentences exchanged in about a minute. The characters have twice the depth and development as most anime characters with half the script. It shows and lets you feel and experience rather than beat you over the head in a Kojima-esque way, and actually requires participation from the viewer rather than just passive absorption. That is the brilliance of Cowboy Bebop. Damn, maybe I just want to go watch that again....
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