1590s, "undo from a fixed position," from un- (2) "reverse, opposite of" + settle (v.). Of the mind, feelings, etc., attested from 1640s. Related: Unsettled; unsettling.
unseemly
unseen
unselfish
unsentimental
unseparable
unsettle
unsettled
unsex
unshakable
unshaken
unsheathe