I finally managed to get Villain by stealing the money from Unnis, tho I had to get the shapeshifter mask first from Wendigo since she doesn't talk to humans. It seems to me it doesn't matter what you do inside Fort Joy. Unnis seems to be the only person to guarantee the Villain tag.
Also, has anyone else noticed how buggy it is to electrify surfaces/clouds? I have to quicksave every time I do it.