Too much Kirby metal. Of course, I like Sakuraba's version.
I haven't heard the entire soundtrack, but the Dark World remix really did it for me. Just reminded me how little LttP gets acknowledged over the years in so many ways when a classic song like the dark world doesn't get a formal remix until recently (with the PH trailer and all). The only LttP songs that pop up in Zelda games now are the ones OoT snatched.
Other mentionables:
Angel Island Zone
All the Metroid tracks
Oot Medley
Space Armada
Tag - "No trolling on my watch!"