While I agree that Sephiroth has a presence like few other villains whom I've seen, I typically find others more
interesting in terms of their motivations (not that there's anything wrong with VII's iconic antagonist, mind
you).
I haven't seen it pop up too too much yet - for which I'm actually greatful, lest it grow too tiresome too
quickly - but I rather enjoy the Ghaleon archetype as it's developed over the years (I term it such because I see
in him the roots of later characters like Krelian and Seymour and their ilk). I'm not saying it's the deepest
thing ever or anything, but I at least find it more compelling personally.
Kefka, though, I thought was interesting for his raw, unabashed madness; they didn't even seem to be hiding it,
from I've seen of the game, and I did kind of enjoy that. He felt a little different from the sorts to whom
I'm usually accustomed.
But to generalize, the sorts of villains I typically enjoy the most are those are are complex and interesting - more
like actual human beings - as opposed to those who are mindlessly evil for evil's sake (though I do think that they
have their place as well). One of the things that draws me to the original (UC timeline) Gundam universe is that, once
you get past the myriad anime cliches and inanities, neither side comes across (I think) as purely good or purely bad; they're some of the best approximations of real world nations
that I've seen, if still very much simplified.
Solidus was also a brilliant example of this, I thought, sans the painfully forced 'history' between him and
Raiden that the writers threw in at the last second; but if I understand his core motivations correctly, and what he
wanted to accomplish, I'd he rooting for the guy.
The long and the short of it is that I essentially prefer antagonists who make you think a bit, and raise interesting
moral questions. For me, they're far and away the most compelling.