The departure comes quite suddenly, given that more seemed to be in store for Harley’s character Logan, who only came to the show in August, 2021.
He had just begun a relationship with fellow character Mackenzie Booth, played by Emily Weir, and teaser trailers for the upcoming season showed a mysterious stranger, known to Logan, would be coming onto the show.
However, it is believed the role of Logan will not be recast.
Harley is now the second person to leave the show since Seven West Media introduced a COVID-19 vaccination mandate on cast and crew.
An email was sent out last October by Director of Production, Andrew Backwell, which said the network would "only engage fully vaccinated presenters, cast, and crew".
It is believed that Harley is not vaccinated against COVID-19.
Sam Frost, who played Jasmine Delaney on the show, will also not be returning.
While there was talk of plans in place for Jasmine to temporarily leave the show while Sam underwent surgery that would in turn allow her to be vaccinated, she has now decided to not return.
However, her exit was reported to be unrelated to the mandate.
Harley excitedly introduced his role on Instagram when Logan first appeared on the show.
"Stoked to finally introduce the Doc! Big thanks and congrats to the whole team @homeandaway," he wrote alongside a picture of himself as Logan.
"What a gig! 🙏🏽🙏🏽."
Aside from Home and Away, Harley is best known for playing Josh Willis in Neighbours between 2013 and 2016.
He pursued acting in America after departing Neighbours, living in Los Angeles with his partner, Natalie Roser, for a number of years.
The actor has also starred in the likes of House Husbands and True Story with Hamish & Andy.