I am with FlareKnight on this with Ultear. Unlike the others who have joined Fairy Tail (including Gemini, Aries, and Virgo), Ultear has been a mastermind and plotter. She seems beyond redemption.
As for Meldy, she just does not fit the "I am evil" look or actions so far. Hence, she appears as a likely candidate to join. She is also cute, so that helps.
As for Capricorn... It is quite obvious, unless Fairy Tail pulls a fast one on us.
I would have thought Mest might have been a candidate as well, due to his goofiness. However, since he is a council member (I guess magical strength is not a requirement of them), I doubt he will join Fairy Tail.
I still think Zeref joining them would be quite a twist. The ultimate evil mage turning a new leaf.
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