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Not sure how many hearts you need for an exp increase, but I noticed my Jolteon found it easier to dodge attacks and land critical hits more often at 4 hearts (though these effects aren't around during double/triple/rotation/online battles, at least I don't think they are...could be wrong)
Anyway, just feed them till they refuse any more poke puffs; play a couple of Amie mini-games and repeat. Got 5 hearts in 20 minutes