It's understood the role will not be recast.
A Seven spokeswoman told The Telegraph in a statement that the network "can confirm Harley will not return to Home and Away when filming returns in the coming weeks".
"Harley leaves with our best wishes and sincere thanks for his work on the show," she added.
The 30-year-old had previously said he felt "very much at home" on the show and was "enjoying every minute of it".
Bonner's departure comes off the back of Frost's, who filmed her last episode as character Jasmine Miles in December.
The 32-year-old revealed in an emotional video on her Instagram in early October that she had not been vaccinated against the coronavirus.
She said she "could get into trouble" for revealing her stance on the vaccine, but pleaded for "compassion" and "empathy" for those who have made the same decision as her.
"It's a really hard time to be in society right now, you feel like you are less of a human and you feel like people judge you, and you're too scared to talk about your opinion or your feelings, and part of you wants to go, 'Well, it's none of your damn business why I'm not [vaccinated]'," she said.
The backlash was swift and ferocious, with many asking how exactly Frost was able to keep working on Home and Away despite not being vaccinated. The former Bachelorette later revealed her character was being "written out" temporarily to allow for her to get the jab.
It was then confirmed she would cut ties with the soap, which she had starred in since 2017.
"We support and respect Sam's decision to leave Home and Away," a Seven statement regarding Frost's departure said.
"Sam leaves with our sincere thanks and very best wishes for the future."
