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Pretty much all of the Zankyou no Terror soundtrack is amazing, VON however is my top pick
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cowboy bebop had a fantastic track and the ending has such a great vibe.
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More recently I really enjoyed the music in Gundam Thunderbolt. Very sad and emotional series, the tracks fit so well.
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Cannot forget Nujabes. Samurai champloo was the first anime I ever watched (excluding pokemon/dbz), the instrumentals throughout were very emotional and memorable. Giving the scenes more life. The show introduced me to anime and nujabes music, forever one of my favourates. Definitely check his stuff out. RIP Nujabes.
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Death note had some very powerful music and Naruto had many OP/ED's that I really enjoyed. FMA:B first opening sticks in my head as one of the tops. Aswell as the opening for GitS SAC.
My favourite anime song of all time is Scattered Rain from Trigun. Now I stress that you HAVE TO listen to the entire thing. I don't care if you think it's a waste of 5:30 of your life.
Hmmm, for openings and endings, here are a few that I like that maybe people haven't seen too much of (though I'm just speculating, not actually sure haha)
New Game Ending: Now Loading!! by fourfolium
I love almost all the Idolmaster songs but here's one I guess
or another. I dunno if anybody's gonna listen anyway, haha.
Inner Universe by Origa, from Ghost In the Shell: Stand Alone Complex, is an absolutely fantastic OP that chills my blood and gets me every time with its beautiful vocals and graceful-sounding melody.
Complications by ROOKiEZ is PUNK'D, the second OP of Durarara!!, will forever remain one of my all-time favourites. Being my favourite OP from my top anime, it's pretty self-explanatory.
I cannot get away with posting this without mentioning My Dearest by supercell. The first OP from Guilty Crown is simply too beautiful to leave out.
In my experience, out of all the anime I've seen over the years, Shigurui stands out as a visceral, cerebral, bloody, gory mess of human greed, envy, feebleness and frailness. It's a look into the lives of a select few samurai and ronin and the madness that binds them together. The artistic style and vibrant style of the show is stunningly beautiful as well as horrifyingly brutal.
Shigurui shows the true way of a samurai, and that sword battles were not a game. To use a real sword was to mean death for you or your opponent. There was no middle ground. A flash of steel, a sweep or jab means instant death. There is no smashing blades against shields. No clashing of sabres or swords to prove your worth or show off your fancy footwork. There are no dragons or daemons to be slain. No princess to be rescued, nor does the world require a hero to save it. In a duel between samurai, you either die, or do not. That is the sum of all things.
The series is short lived, but full in it's delivery.It didn't waste a second of animation and presented itself fully. Everyone that enjoys anime and loves the culture and history of the ancient samurai owes it to themselves to watch Shigurui: Death Frenzy.