The pair are set to move to Halesowen Town having spent the past eight years at Keys Park.
Smith, who recently passed 350 games in-charge of the Pitmen, said: “It is with a heavy heart that with immediate effect Larry and I have tendered our resignations as managers of Hednesford Town Football Club.
“We have had six wonderful years with this fantastic club, and have made some lifelong friends along the way.
“The supporters have always been fantastic with us, but the time is right now for the Club to give someone else the opportunity and for us to start a new chapter in our careers.
“The gates have been low this season, so I would urge all supporters to get behind the Club more than ever now, and get behind the people at the Club who continue to do so much. The time we have had at Hednesford will live with me forever.”
The club added: “Everyone associated with Hednesford Town Football Club would like to place on record their thanks to the management team for the many memorable moments which we have enjoyed during their two spells at Keys Park and we wish them every success in their new appointments.
First Team Coach Francino Francis will take charge of first team affairs while successors to Smith and Chambers are sought.
Their last game in charge was the 1-1 draw at home to Mickleover Sports on Saturday, when the visitors rescued a point thanks to a last minute Nathan Jarman penalty.
They travel to Workington in the EVO-STIK League Premier Division on Saturday.
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