D.Gray-man, Code Geass, and Gankutsuou. X3 Especially Gankutsuou, since the the way they do textures can scare some people off. But it's FANTASTIC. Re-imagined "Count of Monte Cristo" in a futuristic setting. It's gorgeous and well acted and mind-bending and and and and... *flails*
I don't have anyone from the series I want to play, but it's one of my top 10 favorite anime. The fandom is tiny, as far as I know. But every so often you get beautiful cosplay.