Both Smith and Chambers left the Bucks in June, in a shake-up which also saw club chairman Ian Dosser leave.
The pair were replaced by ex-Wolves man Rob Edwards, who has so far guided the club to 14th in the National League North.
Hednesford parted ways with Tooth only seven games into the season and have moved fast to bring back Smith and Chambers, who had a spell at Keys Park between 2010 and 2015.
Smith helped guide the club to the Conference North during his previous tenure as boss, as well as masterminding successes in the Southern League Cup, Birmingham Senior Cup and Staffordshire Senior Cup.
He expressed his happiness at returning to his former club, claiming it was an opportunity he couldn't turn down.
"It is obviously a massive surprise for us how quickly this has all happened. I still have a lot of feelings for this football club, even when I wasn’t involved, and when the chance came to return I couldn’t turn it down." he said.
"I really can’t wait to get going now and we will be working towards Saturday’s game straight away."
Smith and Chambers take on Sutton Coldfield Town this weekend in their first game in charge, hoping to bounce back from two straight 2-0 defeats.