But Remilia and Flandre aren't really villains... Remilia just wants to be able to walk outside during the day (which she can do anyway, but that's besides the point), and Flandre is insane but not evil.
Other than the PC-98 characters like Mima and Shinki, the only real villain is Utsuho, and she's not particularly intelligent.
But I can't really talk, I posted Tenshi earlier :P