The 48-year-old takes charge of the National League Latics after eight years with Everton as Under-23s manager and director of the Premier League club's academy.
The former defender also took charge of the Toffees' first team on a couple of occasions, overseeing the final game of the 2015/16 campaign and for a month during the 2017/18 season.
Unsworth told Oldham's website: "This is the perfect job for me and I'm hugely excited to be joining the club at this time. "I've had opportunities to become a first-team manager at a number of clubs over the past three of four years but they haven't felt quite right. "I genuinely think this club is a sleeping giant, one that can climb up not just one league, but two or three, in a short space of time."
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