For me, I think it'd be this^ song. The song itself combined with what's going on while the song plays... It was the only time throughout Twilight Princess or any other modern Zelda game really, where I actually thought that a character besides the villain might die.
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I love that game Running across Hyrule field in the rain as a wolf while midna was dying was awesome
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It really is a great game, I just wish that enemy and boss difficulty was a higher, the Twilight Realm looked a little better, and that there was more to do out in Hyrule Field just because it's such a nice part of the game. Overall it had my favorite sword combat, my favorite art style (along with OoT and MM) and EASILY my favorite AI companion character in any Zelda game, hell one of my favorite characters in ANY game really.
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Yeah. I was really hoping SS would be what TP could have been It certainly wasn't. I still hope Zelda on Wii U is the game that OoT and TP tried to be. I would be a Wii U for that