The crossword solution for the term 'Smiles Villainously' is 'Sneers'. Sneering is a facial expression that conveys contempt, scorn, or derision. It is often used to express disdain or disapproval of someone or something. It is usually done by curling one's lip and raising one corner of the mouth. Sneering can also be done with words, such as when someone speaks in a mocking or sarcastic tone.