Twilight Princess by far, for me. It seemed to fit everything so much more than music from any other game. Like when entering a new place, Lake Hylia for instance, I'd always think "YES, this is what Lake Hylia should sound like".

The songs might not be catchy and upbeat all the time, like in certain previous games, but they filled each place with more emotion and gave every location a lot of character, in my opinion.

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