Villains who are definitely Merfolk: man/fish hybrids, such as gillmen and mermaids. Unlike in many modern portrayals of mermaids (such as Disney's The Little Mermaid), merfolk are popularly portrayed as evil monsters in folklore, shown to attack and eat people by drowning them underwater in many horror movies such as She Creature and The Creature from the Black Lagoon.
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Ursula (Disney) -
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Maccus
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Maria (Mermaid Melody)
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Marina Del Rey
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Morgana (Disney)
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The Lake Monster (Sailor Moon)
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The Queen of the Black Puddle
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The Queen of the Lair
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The Sorceress (The Little Mermaid)
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The Trench
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The Trench (DC Extended Universe)
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The Witch (Bubble Guppies)
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