The retired midfielder parted ways with the Buccaneers at the end of the 2015/16 campaign.
The Chilli Boys have since announced that Moloi has replaced Mbuyiselo Sambu as head coach Dan Malesela's assistant.
Malesela and Moloi played together at Pirates in the 80's and early 90's.
"I would like to welcome Teboho Moloi to the Chippa United Family," Chippa chairman Siviwe Mpengesi told the club's official website.
“We did not think twice as Management when his name was recommended by the coach," he continued.
“We are confident that their reunion can only take this football Club to greater heights,” he added.
“I would like to wish Mr Moloi all the best during his time with us,” Mpengesi concluded.