Definitely, System Shock 2- the adrenaline-pumping techno music that kicks in when you open the door and get attacked by your first zombies was amazing. I had to switch off the game and wait 24 hours to get the courage to go back into it.
Secret of Mana an old Squaresoft SNES RPG game also had nice music, rather SS2-ish in the penultimate boss battle too.
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