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The original House of the Dead has perhaps the creepiest atmosphere of the bunch, with less cartoonish-looking dismemberment of enemies compared to parts 2 and 3, and zombie designs in the early stages that don't look nearly as gimmicky as what comes later in the series, helping remind the player that these things used to be ordinary people. Their moans and screams also sound a lot less human in this one.
The zombies and bosses in the fourth game. EspeciallyJustice. To elaborate, one of Justice's attacks involve grabbing you, and you have to shake the SMG fast in order to break free of his grasp or he will lick you For Massive Damage. The lovelyclose-up of his face, especially with that tongue... *shudder*
The Empress is a close second, being a gigantic yet very fast creature with dark blue skin and glowing red eyes on an otherwise featureless face, wielding a double-ended chainsaw it uses to cut apart the subway cars James and Kate are trapped on.
The arcade version of Zombie Sophie from the first can be really terrifying.
And in the second and fourth games, Zombie Goldman.
One of The Fool's attacks consists of him shaking up the cage and raining his meal, which is horribly mutilated corpses, down upon you. Most of which will damage you if you don't shoot them out of the way.
In Overkill's final chapter, not only is Varla's brain swapped out for that of Clement's mother, it's plainly visible from the back; not only is a good chunk of her scalp missing, so is part of her cranium!
Meat Katie from Overkill, a mutated butcher who has transformed into a minotaur (with a steer skull for a face!) wielding a giant knife. Even more disturbing than the creature is its death, falling head first into its own meat grinder.
Also from Overkill, the Crawler, a giant, mantis-like mutant fought on top of a train. During the fight, it will hop off the train into the forest on either side. You'll look around, only to find it right next to you, ready to attack.