Probably Calling to the Night. Beautiful =)
I like Final Destination, King Dedede's theme, the SMB3 Airship theme, the Song of Storms, the song from the Wilds level with Marth, Meta, and Ike, (I forget it's name, but it's so catchy!) Tabuu's theme, Gourmet Race, and Route 209.
Recently the 02 remix has grown on me, I didn't like it at first.
Ike's theme is my favorite. It reminds me of a cool part in the game where they took it.
final destination for the win