1540s, "in an unfortunate manner, by ill-fortune," from unfortunate + -ly (2). The original meaning is now rare; the main modern sense of "sad to say, unhappily, unluckily," in parenthetical use, is recorded from 1770s.
unfortunately it rained all day
unforgiven
unforgiving
unforgotten
unformed
unfortunate
unfortunately
unfortune
unfounded
unfree
unfrequented
unfriend