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If I had to narrow it down to three:
Kuroko no Basuke OP1 - Granrodeo: "Can Do"
Psycho-Pass OP - Ling Tosite Sigure: "abnormalize"
Tasogare Otome x Amnesia OP - Konomi Suzuki: "Choir Jail"
Hunter x Hunter 2011 ED2 - Galneryus: "Hunting for your Dreams"
Shin Sekai Yori ED - Risa Taneda: "Wareta Ringo"
Tasogare Otome x Amnesia ED - Aki Okui: "Calender"
Honorable mentions and I had a really difficult time picking the three EDs:
Binbougami ga! OP - Piko: "make my Day!"
Jinrui wa Suitai Shimashita OP - nano.RIPE: "Real World"
Beelzebub ED5 - 9nine: "Shoujo Traveler"
Kingdom ED1 - Takumi Ishida: "Voice of Soul"
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