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Vio wants to understand things. He wants to know why things are what they are, why things do what they do, how they get worse and how they get better.
He also desperately wants to understand himself.
He knows that he felt things, back in the Fire Temple. He knows that he felt bad for tricking his siblings, and for betraying Shadow. He knows that he cared about Shadow, and that he didn’t want to hurt him.
Those feelings just never affected what he did.
As far as he knows, people usually don’t try to kill their friends for any reason. Vio believes that he was Shadow’s friend. He believes that he would have gone with a plan that would have saved Shadow. He just never tried to find one. He never connected the wires between I need to stop Vaati and Ganon and save Zelda, stopping them requires breaking the mirror, and I don’t want to kill Shadow.
Even with Zelda, he didn’t try to save her because he cares, even though he does. He tried to save her because Link wanted to save her, because the one thing that united them was Zelda, because he needed to save her for the story to end.
Heroes save princesses. Heroes kill villains. Vio’s mind had slipped into a storybook, and he was only able to get out of it once the story was over. And the story, for him, was over when Shadow died.
But now, Vio will rewrite this story, whatever it takes. And that starts by understanding.