As should be expected, an epic series like One Piece deserves an epic soundtrack.
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Nothing beats the original opening song, "We Are!", by Hiroshi Kitadani. While One Piece has many great opening and ending songs, this is the only one that sounds apart from mainstream J-music, and more like something specifically written for the show (it was composed by Kouhei Tanaka, after all). It's cheery, upbeat, and has a great singer, and the accompanying animation is impressive. And if you've been a fan of the series for so long and look back upon it, it's bound to strike a few chords in your heart.
The version with all the Straw Hats singing together is even better, turning it into Heartwarming Music. (There really should be a page for that.)
It even makes it into an instrumental, one of the best in the series. It usually plays after the Big Bad is taken down, and everyone's having a good time in the aftermath. Fittingly, it's called, "We did it-Party!"
The 12th opening, "Kaze wo Sagashite" ("Search for the Wind") definitely upholds the standard for great One Piece music. In addition, the TV version is accompanied with epic animation to set up for the Marineford Arc.
If we must speak of the new One Piece songs, we must not soon forget the 13th opening: "One Day" by The ROOTLESS. It fits the epic and tense feel of the Marineford saga perfectly, and also describes the brotherly relationship between Luffy and Ace quite nicely.
Not just the second part, but the rest of the theme as well. Hell, all of the Straw Hats' themes are awesome, and fit them to a T. Sanji's is jazzy and suave, Robin's is sexy, classy and elegant, Usopp's is fast-paced and upbeat, Nami's is cute and mischievous, Zoro's is dark and serious, Franky's is triumphant and awesome (So awesome it was even used before Franky was introduced), Brook's starts off creepy, then becomes goofy and happy, mirroring people's reactions to him (At first they're scared, then realize that Brook is a Nice Guy), Luffy's is adventurous, and Chopper's is cute and happy, curious even.
"Karakuri Castle, Transform" is arguably one of the most intense, fast-paced fight themes in any show, and especially by anime's standards. Played often through the series, KCT makes any scene that much more thrilling.
"Overtaken" makes any scene in which it's played instantly better, because it's usually when the Straw Hats have decided that, no matter how much punishment they've taken already, no matter how hopeless the situation has become, no matter how powerful the Big Bad is, these guys will not back down, they will not surrender, they will pull out all the stops and won't quit until they're dead or have put the villains in their place.
If Overtaken has come on, you know the Mugiwara/Straw Hat Pirates have just officially declared that SOMEONE is about to get their shit DESTROYED.
It's not Dvorak, but the piece that plays during that scene's recreation in Movie 8 (and later on in the actual anime for Rob Lucci's defeat), "I Will Surpass You!", has a wonderful build-up of pain and sorrow before exploding in a triumphant and furious climax as Luffy puts everything he has into his last move to defeat the Big Bad.
While it started out as a funny gag song, (warning, clip arguably has some spoiler material prior to Enies Lobby) "The Man from the Island of Snipers" becomes Awesome Music when Usopp gets dangerous. After all, this is a series about fulfilling one's dreams — so what is more badass in context than a song about one's dream self?
The most terrifying combination of music when played to the presence of someone like Bartholomew Kuma has to be Desperate Situation and Difficult until 1:50. If either one of those pieces are playing, it's usually a sign that shit has hit the fan.
The music at the end of the most recent episodes as Oars, dying, reaches out to Ace is the most amazing, heart-rending piece the recent episodes. It's called "Dokuro ga Shinnen no Shouchou", and is from the 9th Movie Soundtrack.
Dokuro wa Shinnen no Shouchou from the 9th Movie. Notable moments when this song played during the anime includes the part in Impel Down where Luffy tells Iva that he's going to Marineford to rescue Ace and, more memorably, the scene where Whitebeard makes an epic Last Stand against the marines.
The second part from The World's Number One Oden Store is an amazingly beautiful track, and does a great job of getting across the great things that tend to happen in One Piece flashbacks (Saul's betrayal of the marines and Roger/Rayleigh's first meetings stand out).
Karakuri Defense System, Deploy is the kind of theme that makes any dramatic scene twice as intense. Usually played whenever the bad guy has the upper hand in a fight, or when there's impending doom.
The song that plays in various flashbacks (such as the barkeep's reminiscence of Gold Roger) is particularly great, providing a trailer-esque quality to the flashbacks, and sounding great on its own.