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Agree with you on Baccano's Opening (Guns & Roses), OP! It's definitely one of my top ten! This is really hard though... So. Many.
Openings:
Spirit Inspiration by Nano from Btooom!
Resonance by TM Revolution from Soul Eater
Rose-Hip Bullet by Granrodeo from Togainu no Chi
Bloody Stream by Coda from Jojo's Bizarre Adventures (the new anime)
Rewrite by Asian Kung-fu Generation from Fullmetal Alchemist
Endings:
Real Folk Blues by Vitamenless from Cowboy Bebop
Shiki no Uta (Song of Four Seasons) by Shik (ft. MINMI) from Samurai Champloo
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