Soloman Lane from Mission: Impossible-Rouge Nation and Mission: Impossible-Fallout.
Cayden James from Arrow.
Michael from The Good Place.
Edward Nygma/The Riddler from Gotham.
Professor Gerald Robotnik from Sonic the Hedgehog.
Dawn Bellwether from Zootopia.
Justin Hammer from Iron Man 2.
Arnim Zola from the Marvel Cinematic Universe.
Phoenix Buchanan from Paddington 2.
Mr. Reed from Heretic.
Ally Allston from Superman & Lois.
Pollux Troy from Face/Off.
Richmond Valentine from Kingsman: The Secret Service.
Dean Armitage from Get Out.
Wedgie Woman.
Melvin Sneedly.
Professor Poopypants.
Qilby from Wakfu (before his 'villain form')
Merely Eggman, easy!
Bad Cop (The Lego Movie)
Dr. Finkelstein (The Nightmare Before Christmas)
Dwayne LaFontant (Over the Hedge)
Honest John (Pinocchio, albeit in only one scene)
King Malbert (Igor, albeit they're sunglasses)
Mr. Crocker (The Fairly Oddparents)
Professor Z. (Cars 2, albeit it's a monocle)
Mortmottimes and Derridommis (In Search of Santa, albeit the latter also wears a monocle)
Vector Perkins (Despicable Me)
Doctor Ivo Robotnik, any version of Baxter Stockman, Aizen, Android 21.
Herbert West
Carol from The Loud House
Gendo Ikari
Dr. Herman Varnick from Beethoven
Professor Finbarr Calamitous from The Adventures of Jimmy Neutron: Boy Genius
Professor Cog from Power Rangers Super Samurai and Power Rangers Super Megaforce.
What do you think?