Well.. for me since I play all games with headphones FEAR was the worst.. that damn music made your hairs stand on end and when you caught movement out of the corner of your eye it was like "WTF!!!!" and mouse spins around aimlessly and you hit full reverse shooting like a wildman lol...
But a few games have really captured the mood with music or just used the typical "when player gets to spot X, we make nasty mcbadguy jump out of spot y and lay the boots to him)" Far Cry was good for that.. damn monkies