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Of the ones on this poll, definitely Mesprit. It requires a long, involved strategy unique to itself (besides Cresselia). Unless you use a Master Ball.
Mesprit was hard for me. I used mean look on it, but it took me over 50 Ultra Balls.
Azelf and Uxie were very easy. 7 Dusk balls each if I remember properly.
The Lake Spirits seemed to give me the most trouble. Mespirit was annoying, but it wasn't too hard once I got my Gallade with mean look, false swipe, and hypnosis. I think Azelf was the most frustrating for me, pretty sure I restarted a few times because I kept running out of pokeballs.
For me, Mesprit was the hardest to catch. I didn't want to use my Master Balls (yes, balls, as in plural. More than one) on Mesprit because I was saving them. It kept either running away for killing my Golbat (the only Poke I had w/ Mean Look and stat decreasing moves.) After about 3 hours of looking for it, I caught it...damn Mesprit.
I would say mesprit becuase becuase it would escaping, and I had to trade for a golbat with mean look. Giratina was a little tricky for me though. Heatran, Dialga, Palkia was pretty easy.
Giratina was a royal pain for me, I had to throw so many Dusk, Timer and Ultra balls I may have an olympic record for it. He was so awkward to catch i decided to keep it in my squad and make it hate me so it was mutual.