Sion's new Lore is really good, especially if you look at some of the design documents that went with it that point out some of the interesting details of his body. His jaw is Jarvan I's crown, for example, and his shoulder armor is deliberately meant to resemble Darius' because he was the original Hand Of Noxus. The detail work is just nice.
I was also a big fan of old Warwick, back when it was Soraka's curse that turned him from a master chemist to a werewolf. I liked that one a little better because instead of trying to fix it, he embraced it and just decided to start attacking people up close with claws instead of far away with bombs. Warwick was always a monster, all Soraka accomplished was making him look like one. I thought that characterized him really well.
I'm a fan of Blitzcrank too. Big robot just trying to find his way in the world.