For me, it's SUPER FUCKING METROID. Those songs fucking blew my mind. The variety of them and how well they suited the environment/situations are perfect. The title screen sets the mood with the eerie tune, the corpses bathed in the glow of the consoles, the rhythmic cooing of the metroid hatchling. And it only goes uphill from there.
Here's a sample for you. This is the track that plays when you travel to the Wrecked Ship, feeling like hot shit because you just got the Grapple Beam and the song makes you feel strong. Then what happens? You get into the destroyed spacecraft and the music is replaced by an unsettling atmosphere-creating track that taunts you as you uneasily make your way through the strange craft, taking damage from exposed wires and fighting things you've never seen before.
TL;DR, SUPER FUCKING METROID
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