Armando Salazar - Javier Bardem
The Pirate of the Caribbean franchise had a lot of CGI involved. A lot of the undead pirates relied on heavy post-production to make them look realistically zombified. Armando Salazer, played by Javier Bardem, was the main villain in Dead Men Tell No Tales as he tried to murder Jack Sparrow. Bardem's preparation for the role took three hours every time they had to film.
Pinhead - Doug Bradley
Pinhead is the main villain in the Hellraiser franchise. Doug Bradley played the main Cenobite (extra-dimensional beings who are mutilated and brainwashed into torturing humans for all eternity in the Labyrinth) from 1987 until 2005. He finally turned down a role after he felt like the films had been played out and that it was just a cheap cash grab.