I really like all these suggestions. (Yeah, I read them all.)
I'd just like to say something though. Our characters have attached fingers. It's like they are all wearing mittens.
Unless this gets changed (and it most likely will not) there will be no pointing of any kind. Also, any sort of facial contortion (smiling, smirking, brow-raising, etc.) will not happen.
On to my suggestions.
We need walking. Like someone said before, my supervillain does not run. He's too important for that.
More intensely angry poses.
An "Evil Ash" taunt dance. Who isn't going to make evil-Synapse, evil-Positron, and even... evil-Statesman?
Laughing that turns into a fit of coughing. Those people with the old man face should act like old men.
Stomp foot, then swivel it back and forth as if crushing an insect. Very dramatic.
