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Well I can't think of five so I'll just talk about my favorite one...
Personally, my all time favorite is the Cowboy Bebop soundtrack. Yoko Kanno did a crazy awesome job with it. You don't have to be a fan of Cowboy Bebop to like it, I told a non-anime fan friend of mine to check it out and he really enjoyed it.
Shinichiro Watanabe was just genius in his execution of Kanno's work. I was reading an interview with Watanabe about a year ago and he said that he picked the music first, then animated the scenes to the music.
Generally, when I watch anime the music plays a secondary role in the anime. However, in Cowboy Bebop it really plays a primary role, it's just great.
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