Gould was unveiled as one fo SuperSport’s new signings at their awards ceremony on Thursday night.
The 33-year-old returns to Matsatsantsa after an injury-plagued four years spent at Naturena and adds to the defensive stocks of coach Stuart Baxter.
Gould was part of the squad for all three of Baxter’s seasons at Chiefs, but saw his opportunities limited by two serious injuries.
Gould made 117 starts during his first spell with Matsatsantsa between 2008 and 2012, when he won two league titles and the Nedbank Cup.
He was released by Chiefs at the end of last season and had been training with SuperSport for some weeks before being signed.
Gould made his PSL debut in the 2001/02 season at Jomo Cosmos and has 272 starts in the South African top-flight.