And a few honorable mentions for my own satisfaction include: Schindler's List, HaraKiri, Saving Private Ryan, Memento, The Prestige, Gladiator, The Lion King, A Clockwork Orange, Seven, Ran, Scarface, Halloween, The Thing, Kagemusha, The Twilight Samurai.
I'm level 97; still in my first playthrough, so I haven't seen all the bosses yet admittedly. But so far the ones I have played against have all seemed uninspired and generic looking compared to the other two games. I don't know if it's because the majority of them are all humanoid looking or not, but they all sure do look the damn same. I'm hoping I'm still early enough in the game that they're saving their manus, kalameet and artorias equivalents until later.
Silent Hill on the PSX was the first game to truly unnerve me, and scare me enough that I didn't want to progress to the next area. Resident Evil (before Remake came out) never had the same effect on me, and was more of an atmospheric experience for me.