I can't think of many at the moment, but two that stick out for me are:
Zelda: Ocarina of Time (N64 version) with Ganon. Perfect atmosphere and my personal favorite Ganon by far.
Castlevania: Dawn of Sorrow's final boss for just how epic and bloody it was despite being a T rated game. Giant monster made from the flesh and bone of fallen enemies? Incredible.
OT: Saren. Maybe not so much the battle so much as the character. You could have a pretty hard fight if you wanted, but it really showed Saren as a tragic and conflicted character.
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