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For me personally?

Sakura Haibara in Fatal Frame 4.

She's unique in that while she's terrifying, her character almost entirely sympathetic. She's not evil or sadistic, or cruel, she's simply a tortured soul who wreaks slaughter because simply to look at her is fatal. Her backstory is quite sad; she's suffering from a disease that's basically a supernatural stand-in for Alzheimers, and is losing her memories and with them her very identity. She volunteers to be part of a ceremony designed to lift the curse, but when it fails she is turned into a walking deliverer of death who wanders the island until nobody is left alive.

The times you encounter her in the game are absolutely blood-curdling, as the screen turns black and white with Sakura little more than a dark shape surrounding by burning white fires, the soundtrack filled with eerie keening.

No other video game character has made me lose a night of sleep.