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Here's my personal theory on which of the Elements of Harmony Celestia and Luna wielded at one time:
- Luna: Generosity, Honesty, Loyalty.
- Celestia: Kindness, Laughter, Magic.
Why do I think that? Well, from what I've seen, Luna had a difficult time making friends, she doesn't strike me as a liar, and laughter did not see to come naturally for her. She seems to be as honest as they come, and she seemed to be displeased with how other ponies seemed to repay her loyalty and generosity with nothing. Kindness does not seem to come easity to her, either.
Celestia has a natural sense of humour, is generally kind, and seems to make friends without too much of a problem. She has shown herself to be devious, which would go against honesty. I'm not sure how much generosity and loyalty she has.
Now, this is just my theory. I'm wondering what your thoughts are on this.