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Although I dropped Watamote almost right away haha the OP was pretty good. Also Anohana's OP will always be a favorite <3 The Gintama ones are sound pretty solid, I promise I will get to watching it eventually ;~;
Any and all of the openings to the various series of Sayonara Zetsubou Sensei. They're all extremely catchy, sung by the cast of the show, and the accompanying animation is utterly messed-up to varying degrees:
Boys & Girls by LMC. Second Katekyo Hitman Reborn opening.
Hajimari no Sora, 11th Fairy Tail opening if I remember right. Aaaand then there's Masayume Chasing, the newest Fairy Tail (2014) opening.
..can't forget the first Soul Eater opening either omg. :DDD These four are my top four and I flip-flop on which I prefer since it depends on my mood at the time.
I really really like the 2nd Opening to Kill la Kill! It's soooooo gooooddddd. I was going to post a link here, but I can't find an opening that isn't pitched :(.