The 35-year-old joined the Students at the start of the campaign following his return from Europe.
However, despite high expectations, Pienaar failed to set the PSL alight, and could do little to help the Johannesburg-based outfit move out of the relegation zone.
"Unfortunately it hasn't worked and we agreed to part ways and we wish him all the best in his future," Hunt was quoted as saying by Independent Media.
This was soon after he left English Premier League side Sunderland, who got relegated at the end of the 2016/17 season.
Reports emerged towards the end of 2016 that Wits were considering terminating Pienaar's contract.
Pienaar, who played for some of the top European teams, including Ajax Amsterdam, Borussia Dortmund and Tottenham Hotspur during his 16-year spell abroad, featured 11 times in all official competitions for Wits with registering a single assist or finding the back of the net.
Meanwhile, Polokwane City have reinforced their squad with the acquisition of central defender Sibusiso Sikhosana from Witbank Spurs and striker Dominic Chungwa from Caps United.
BOOM! We happy to announce addition to our playing personnel— #RiseAndShine (@polokwane_city) January 2, 2018
Central Defender: Sibusiso Sikhosana #33 from Witbank Spurs and Striker: Dominic Chungwa #9 from Caps United
The Limpopo-based side also roped in former Orlando Pirates physical trainer Japhet Borges Neto.
Boom! As promised— #RiseAndShine (@polokwane_city) January 2, 2018
"We welcome Former Orlando Pirates Physical Trainer Japhet Borges Neto into our Technical Team; comes with 10 years wealth of experience in South African Football"