The 31-year-old, who played for Liverpool between 2012 and 2018, will end her stint in the States with Racing Louisville FC to return to England.
In 2013 and 2014, She previously won the WSL titles with Liverpool.
Matt Beard (LFC Women manager) said of Bonner’s arrival: “It was too good an opportunity to pass up to bring Gemma back to the football club.
“We had a great working relationship before and she will bring leadership and experience to the team.
“She’s won everything in England with Liverpool and Man City and has now experienced America to broaden her horizons and open her eyes to different football cultures.
“It just feels like she’s coming home.”
Bonner said on the move: “It’s a pretty special moment for me. I still pinch myself when I’m coming into Anfield.
“I’m super excited to be back and I can’t wait to pull the shirt on again and get out there with the girls — and get back playing for Liverpool.
“I was here for quite a while before, it was a hard decision to leave but I think I always knew within myself that one day I would love to come back to Liverpool. Now the time feels right.
“The team have started the season really well, obviously had a successful season last year getting back into the top league. They’ve got good foundations and are definitely building.
“Hopefully I can come in and contribute to the continued progression.”