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This is a difficult one, but:
For OPs, I'd give first place to Again (Fullmetal Alchemist Brotherhood).
For EDs... gah, it's too close. Maybe Brave Song (Angel Beats).
Other favourites would have to be Joint (Shakugan no Shana II), The World (Death Note), Uragiri no Yuuyake (Durarara), and Toki wo Kizamu Uta (Clannad: After Story).
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