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I'm thinking Umaro or Cyan. to turn an otherwise unuseful character into a high-flying jumpy imp. Also they both sport good physical offence, and can't really be used as mages. If you imp Umaro, can you control him? If not I guess I'll go with Cyan, unless there's a better canadate I'm ignoring.
IIRC, Umaro will still do his char toss attack/blizzard while Imped, if you have the appropriate relics equipped. Jump would be pretty worthless on him though, since you can't give him a spear and I don't think the game would properly recognize his Fight command anyway. If you Imp him all you'd be doing is effectively making his Fight action even worse than it is already.
"Oh man, that is a burn. Dude, you just got burned. Burned, dude. BURNED." "Shut up. Your armor's pink."
Terra and Celes are wasted as Imps, both have good equipment and are proficient with Magic. They don't need it.
Strago and Relm fall in the same boat, but don't have the physical stats to make good use of the Dragoon setup anyway, this applies to Gogo too.
Locke is probably doing more damage with Valiant Knife and Master's Scroll. If you're not using those (or Lightbringer) then he suddenly falls into contention.
Setzer can be outfitted as an imp and still retain his use of Fixed Dice/Master's Scroll, so that's something to consider. If someone else is using the Master's Scroll then yeah, he'd be a good candidate for the Dragoon Boots/Dragon Horn (to better his consistent damage, if nothing else).
Gau and Umaro can't use Dragoon Boots, so that's them out. Umaro can't use any of the imp gear at all, in fact.
Edgar and Mog both have better Jump setups with Holy Lance. In Mog's case, he already reaches max physical defense and has high magic defense with Snow Scarf, so really he'd be trading the use of his skillsets for Water absorption, which is hardly worth it.
So this leaves Sabin, Shadow and Cyan. I wouldn't bother with Shadow, since he can target Throw and his evasion is so high that an Imp's defenses largely don't matter. Sabin...uh...depends if the Jump attacks are outdamaging Phantom Rush. If they are then he makes a good Imp, he could certainly use the extra defenses. Cyan can be an effective Imp too, the Jump setup probably won't be too far behind Tempest in damage, substituting the charge time for being airborne (and invincible, mind) for a few seconds.
tl:dr version - If you're not using their optimal setups for whatever reason, then Sabin, Locke, Setzer and Cyan are probably the best candidates for Imp.
Sabin's the best from a pure stastitical standpoint, I believe, if you're talking purely about Imp Dragoons.
Setzer's the best in practice. Fixed Dice have no losses from Imp, and he only needs one Relic slot (for Master's Scroll) for maximum benefits. Downside is he can't use Ribbon, but no Imp set ups can. Admittedly, as an Imp, you don't care about Silence status, Berserk becomes a POSITIVE status (only for Setzer though; I don't think Berserk transfers to Jump outside of the initial turn, but could bew rong), Blind is meaningless with Fixed Dice (let alone with Master's Scroll) cause they can't miss anyway, Poison and Siezure just aren't threatening enough by themselves. So this leaves Confusion, Instant Death, Petrify and Zombie as the only things to really care about, and 3 of those 4 status are covered by the Safety Bit anyway.
If you don't care about status immunities, Setzer takes it a step further wtih the Black Belt, adding in more hits.
Most characters don't benefit from Imp set ups though. Terra/Celes have too good a draw on equips to bother dropping it, Mog/Edgar gain barely anything worth noting, the loss of variety > the increase in defenses/damage (ESPECIALLY in Mog's case, where he already has 255 Defense), Strago/Relm are just inferior to other options as imps, as they scream "Mages!" (not to mention Relm loses Cat-Ear Hood...)...yeah.
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