I know a lot of những người hâm mộ hate him, but I LOVED Ketch from Supernatural (and I ALWAYS tình yêu Crowley...though I guess he's not so much a villain these days).
Alex Drake, Wren Kingston, Noel Kahn, Mary Drake, and Jenna Marshall from Pretty Little Liars are pretty fantastic. Reiner and Bertoldt from Attack on Titan are great.