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Arceus >< Since Sometimes Infernape one hits him...or sometimes arceus one hits infernape >< took me like 125 Pokeballs and 92 ultras to capture him D:
Mespirit was the most challenging for me. Even when it was paralyzed and almost dead I still could grab it with a quick or dusk ball like I did Cresselia.
Uxie was the hardest to catch for me. I got it down to 1 HP and just kept throwing Ultra Ball after Ultra Ball at it, with an occasional Timer Ball. 4 times I used as many as I could and then it used Struggle and killed itself...:pokeball:
Cresselia. She won't even sit in a ball for ten seconds...and considering the fact that she is a migrating Pokemon...it makes it even harder to catch her!
Giratina is a puzzle I had to figure out. It only had a trickle of HP left while it was sleeping and the PokeBall always plopped back open to reveal the stupid sleeping Giratina.
Giratina on Platinum, definitely. I had him asleep and on one hit point thanks to False Swipe, and I ended up using 35 Poké Balls, 8 Great Balls, 4 Quick Balls and 29 Ultra Balls and not one worked.
Azelf kept powering up and then killing my team with a single Swift attack. I haven't had a chance yet to take on many of the others, so it's the hardest I've attempted to catch.
Cresselia and Mesprit. On Diamond, Cresselia was cake, but on Platinum she cost me hours upon hours of hunting, battling, spamming potions and resetting...
I find that I get really lucky when it comes to roamers so Mespirit,Cresselia,Zapdos,Articuno and Moltres are usually no problem for me but the Pokemon I might always spend hours trying to catch Giratina. It's not really the one in Platinum but the level 70 one in D/P that seems to give me the most problems.
For me, Giratina was hard. Like, really hard... I didn't have a master ball till later and the thing K.Od my Rayquazza, which was about five levels above it. With further calculations, Rayquazza had better defense too.
That moltres in FireRed was a pain, but none of the 4th gen legendaries gave me much trouble. Cresselia was a bit of a pain, but I only needed to SR once so it's all good.