Not a Neon Genesis fan, never even seen it actually, all I know about it is that is an anime. That said, based on the general esthetics of each poster I would say either the first one or the last one. If it were myself, I would probably take the top one, the name of the series or movie or whatever it is at the top of the poster adds something. It is more like a movie poster. I prefer movie posters because in being a movie posters they symbolize and represent the film in its entirety, rather than a still frame or a particular character. For example, let's use Arnie's posters, he has the one of Dath Vader, which would lead someone who sees it to believe that he likes Darth Vader, which is probably true. Next is his Star Wars Trilogy poster with Luke and Vader clashing sabers, this one would indicate to someone that he likes the SW trilogy, which is true. Even though it has both Luke and Vader on it, it doesn't symbolize just a fondness for those two characters, but a fondness for the entire trilogy.

I am not quite sure why I am spouting a long winded explaination of my philosophy on posters, but during the course of writing all this, I have definitely decided I think you should get the third one, Sean. It has more character to it. And seems to fit better with the style of your John Lennon and skull posters.