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From favorite to least favorite, between Nightmare Moon, Discord, Queen Chrysalis, King Sombra,  Sunset Shimmer, and the black vines, and, if you wish, Ahuizotl, Mane-iac, and Windigos? And if you want, you can list Sunset Shimmer and her demon form separately, since they're entirely different types of villain.

For me, it's...

  1. Queen Chrysalis
  2. King Sombra
  3. Discord
  4. Tirek
  5. Nightmare Moon
  6. Mane-iac
  7. Demon Sunset Shimmer
  8. Ahuizotl
  9. Windigos
  10. Trixie
  11. Plunderseeds
  12. Sunset Shimmer

I almost want to tie Discord with Nightmare Moon

Minor antagonists who are more of jerks are not listed here. Recently added Trixie, I make an exception for her since she goes from jerk to evil when corrupted.

By request here's a poll: Of all the main villains, major villains, and minor villains just as evil as any of the main villains, who is your most favorite? (Updated the poll to include the Tatzlwurm, the Chimera, Garble, and Tirek, as well as some of the earlier monsters that try to kill the heroes)

Who is your most favorite of these villains? (Part 2)
 
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The poll was created at 20:49 on May 13, 2014, and so far 11 people voted.

If you still want to see the results of the older poll... Here is is below.

Who is your most favorite of these villains?
 
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The poll was created at 08:12 on January 3, 2014, and so far 26 people voted.