The award did not exist in 1961, so I’ll give my retrospective nominations and vote.
My Nominations: Atlantis, The Lost Continent. The Day The Earth Caught Fire. The Pit And The Pendulum.
Sure, Atlantis is a terrible film famous for its use of stock footage, but the effects are pretty damn good and the make-up is also up to scratch. The Pit And The Pendulum scores another personal nomination for its use of make-up, adding greatly to the darkly gothic feel, while The Day The Earth Caught Fire has a subtle use of make-up to play off the excellent effects. My win goes to Atlantis and the stellar work of William Tuttle and Mary Keats.