Yes, about time a thread started on this.
Personally, I don't think Jeff would work all that well...I mean...he has absolutely no close range physical tricks he can use. I can't imagine him doing kicking and punching and headbutting attacks like Ness...but if perhaps he had some short range weapons for his A attacks, it would work. Here's my moveset for Jeff:
Forward B: bottle rocket- you can hold B to charge it up for more power, but if you hold it for too long, the bottle explodes and Jeff is blown up into the air. He doesn't take damage, but if he is on high %, then he WILL be KO'd. Any enemy caught in the Bottle rocket's Self Destruct explosion gets a massive knockback and about...oooh, 25 damage? In the air, this move makes Jeff "float" for a while, therefore allowing him to use the self destruct for recovery purposes.
B: heavy bazooka- A bit like Yoshi's eggs. The longer you hold B, the higher Jeff aims. Hold B for too long and Jeff puts the bazooka away without firing. About the same damage and knockback as Samus's strong missiles and it fires in a straight trajectory and the actual projectile moves quite fast. However, just tapping B to fire a horizontal shot has reasonable (fair) startup time.
Up B: sheild breaker- (or a different name so as not to be like Marth's SB, it's the item Jeff makes out of a pipe) Jeff jumps throught he air while swinging his sheild breaker in a dolphin slash style ark. The thing is, this gets very little vertical distance, mostly horizontal, making it a poor recovery ability on its own, but coupled with the bottle rocket self destruct, it would allow Jeff to recover in a reverse Luigi fashion. This attack does very little damage but has the same sheild breaking ability as a fan smash attack. (maybe that's a little bit broken, perhaps the same sheild breaking ability as a fan f-tilt then).
Down B: HP sucker- Jeff takes out the weapon (with the startup time of Mewtwo's disable attack) and fires a short ranged electricity beam in front of him. Oh hit, the beam shocks and combos the target for about 13% damage and gives the HP to Jeff as well as knocking the target back in a similar trajectory to Fox's shine. When this move is sheilded or doged, the lag time is really bad, therefore it's not a broken move. In the air, this move makes Jeff fall like a rock, so it can't be used like Fox's shine.
Super attack: Hungry Hungry HP sucker-like the HP sucker, only it hits at long range, targets all characters on screen, and distributes 31% damage between all of them and gives it to Jeff. This means that in one on one battles, this move does 31% to the opponent every time and heals Jeff immensly.
However, I think that I'd rather see Paula.
Forward B: PSI fire- like Ness's PK fire but instead of comboing, this attack blows the opponent up into the air. Can KO.
B: PSI freeze-it charges in a similar fashion to Sheik's needles (but cannot be stored) and when fired, it only travels a short distance. However, on hit, the move freezes the opponent (no damage, but when fully charged, it can get an easy star KO) even uncharged, this move will prop the opponent up high in the air for Paula to toy with. Yes, yes, I know that in Earthbound, PSI freeze was a very powerful move, but hey, they changed PK flash to do damage, so I think that a no-damage freeze attack is justified.
Up B: PSI thunder-yeah, yeah, I honestly can't think of anything better for Paula. It should be Ness's old PK thunder, yes, the one that can easilly cancel people's second jumps and gives a really good boost for recovery.
Down B: PSI sheild-rather than absorb energy attacks, it could absorb energy attacks and then deal GUARANTEED damage to the target like it does in the game. Say Mario shoots a fireball at you, and you use this move, then instantly you see Mario get burned as if he just hit himself with a fireball. That would work nicely, I think.
Super attack: Psi thunder omega: I imagine it to be something like those Japanese robot homing lasers that you see on Gundam anime sometimes. You know, the cool ones that make a funny noise and all these stringy beams of light swarm the target and...yeah, but with thunderballs instead.
Poo is also a possibility, although I honestly don't like him much.
Same moveset as Paula above, because he uses mostly the same PSI as her. Because Poo can get a secret weapon called the King's Sword, his smash attack could involve this sword. His super attack would definately be PSI starstorm. Definately.