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Comics, DC wins easily in quantity and quality.

Movies, they are about tied. Only good villains in the recent movies are
1. Loki
2. Lex Luthor
3. General Zod and of course Faora kicked ass
4. Red Skull
5. Amanda Waller
6. Winter Soldier

Honorable menions include Doomsday (He was strong as F and did his one job, KO'd Supes) Joker (basically a cameo, but I want more).

Shit villains below
1. Enchantress
2. Whatever Iron Man 1's villain was called if he had a name
3. Manaran twist
4. Dude who shot fire out of mouth in Iron Man 3
5. Whip dude from Iron Man 2
6. Malekith from Thor 2
7. Yellowjacket from Ant Man
8. Villain from GoG
9. Zemo from Civil War
10. Crossbones (he wasn't horrible till they ruined him to canon fodder in Civl War
11. Ultron. (looked cool, sounded cool, but was boring as f and stupid plot)

Then there is the mystery Villain. Will Thanos get up from his chair and be a great villain or another Marvel wash away. I mean heck, I don't even know half the villains names in the marvel movies cause they were so forgettable, bad.

Not sure where to put Suicide Squad Members. The story stucked and movie was a mess, but for the most part they rocked their characters. I want to see a lot more of Harley Quinn, Deadshot and Captain Boomerang in future movies. But they were not villains in that movie, so not on above list.