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34 Ulysses Klaue (MCU)
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44 Mysterio (Spider-Man: Far From Home)
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52 Toad (X-Men)
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57 Sandman (Spider-Man 3)
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67 Abomination (The Incredible Hulk)
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65 Nebula (MCU)
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70 Crossbones (MCU)
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71 Electro (The Amazing Spider-Man 2)
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73 Apocalypse (X-Men: Apocalypse)
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74 Kaecilius (Doctor Strange)
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84 Erik Killmonger (Black Panther)
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88 Sabretooth (X-Men Origins: Wolverine)
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96 Calvin Johnson (Agents of S.H.I.E.L.D.)
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98 Justin Hammer (Iron Man 2)
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99 Jasper Sitwell (MCU)
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102 Red Skull (MCU)
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106 Aldrich Killian (Iron Man 3)
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110 Collector (Guardians of the Galaxy)
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113 Yellowjacket (Ant-Man)
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114 Wolfgang von Strucker (Avengers: Age of Ultron)
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121 Grandmaster (Thor: Ragnarok)
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128 Magneto (X-Men films)
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138 Whiplash (Iron Man 2)
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203 Dormammu (Doctor Strange)
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Everyone to post 114 captured. Will update the list in a moment. Loki and zuckyd1 are both out of ammo for now. Everyone else still has 30 rounds.
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24 Ray Krzeminski, Agent Carter
I'd argue he wasn't a villain. A jerk of the highest order, yes, but he was working for the good guys, even if on a personal level he was a sexist boor.
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28 The Other (Thanos' servant), MCU
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56 Mephisto, Ghost Rider: Spirit of Vengeance
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72 Turk Barrett, Netflix Daredevil
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82 John Pilgrim, Netflix Punisher