I feel like I've seen everything awesome in anime already, and I know that's not true, but my well of familiarity has certainly run dry. I'm really hoping there are a few more of those series that can get a few surprised leaps to my feet as clever twists and plots unveil themselves. I really loved Akagi, it wasn't the surprise you kind of intellectual battle story, but instead a great intellectual battle of psyches. Monster was another one that I got the same feel, even though it was a very different theme, the sudden realizations of character motivations that changes the whole story up to that point.
Obviously you see some of this in Code Geass, Deathnote, and of course Hunter X Hunter as well. I particularly am enjoying the newer Hunter X Hunter eps in this regard (and i loved the old ones like crazy too), as I never read too far into the manga. The long-run plans that nen users have to enact to win, and tricks that they put their lives on the line for (even the board game conversations the king has). Gankatsuo was a pretty good one in this regard.
Searching around the forums I tracked a few suggestions which I am currently getting, though I don't know how well they will fall into this-
Fantastic Children, Zetsuen no Tempest, Psycho Pass.
The point is clever characters challenging each other intellectually, preferably with their lives on the line. The seriousness of the stakes are important, though the tone of the series doesn't have to be completely serious. Not really interested in a sports series, ecchi, or anything overly mundane.
Thanks!
My seen anime list-
http://www.anime-planet.com/users/Roaky/anime---
Edit: And I forgot to mention my all time favorite as an example: Legend of Galactic Heroes.