1590s, "not peaceful, not firmly established," from unsettle (v.) or else from un- (1) "not" + past participle of settle (v.). Meaning "not occupied by settlers" is attested from 1724.
an unsettled state of mind
an unsettled issue
an unsettled lifestyle
unsettled weather with rain and hail and sunshine coming one right after the other
unsettled territory
unseen
unselfish
unsentimental
unseparable
unsettle
unsettled
unsex
unshakable
unshaken
unsheathe
unshod