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I've loved a lot of anime OPs! Let's see, my favourites are probably:

Ao no Exorcist OP1 (Core Pride) & OP2 (In My World)
Bleach OP2 (D-tecnoLife) & OP10 (Shōjo S)
Full Metal Alchemist: Brotherhood OP1 (Again)
Death Note OP2 (What's Up, People?!)