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hands down Sengoku Basara. The best/interesting part is that its all in English but sounds foreign thanks to the singers heavy accent. http://www.youtube.com/watch?v=8lRyDrUD8lY&list=FLSLRHFIToEDlOoHcvbjh2WQ&index=1
i also really enjoyed the borderlands (both games) theme songs and Street Fighter x Tekken.... and RE 6. you guys and gals may not like the gameplay of some of my picks, but imo they have amazing theme songs and OST's.