Old Mother in Unearthly Child.
I think Drahvin were mentioned as members of the Alliance.
Frankenstein Monster Robot serves 'Big Bad' in The Chase.
ok... more of an ally really.
Glitz, a villain?
Teselecta, not really
Giles Kent is as much a villain in Enemy Of The World.
Radcliffe in Remembrance.
(TV show only)
The Monk is also listed as Mortimus, which is a book name.