Choosing one single game with the best soundtrack would be impossible. So I will just name a few songs that I find awesome:
The Legend of Zelda:
Ocarina of Time - Fire boss battle, Gerudo Valley, Ganondorf battle
Majora's Mask - Song of Healing
Twilight Princess - Midna's Lament
Skyward Sword - Ghirahim Battle
Super Mario 64 - Bowser stage, credits
Mario Kart 64 - Rainbow Road, credits
Mario Kart: Super Circuit - Sky Garden
Mario Kart 7 - Koopa City
Pokémon Gold/Silver version - Lance/Red Battle
Pokémon Ruby/Sapphire version - Rival Battle
Pokémon Colosseum - Cipher Peon Battle
Halo: CE - Main theme
Halo 3: ODST - Skyline
Halo 4 - Main theme
Metroid Prime 2 - Sanctuary Fortress, Darkness
F-Zero X - Mute City
F-Zero GX - Fire Field, Pico theme
Plus pretty much all OST by Rare ltd.
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