He replaces Ernst Middendorp, who jumped ship at Maritzburg on Thursday to take up the vacant Celtic job.
For Larsen, it is a return to the club where he first began his coaching career as assistant to Gordon Igesund.
The 42-year-old moved to Celtic where he won last year's Telkom Knockout title but quit after a poor start to the new campaign, the final straw being a home thumping by Mamelodi Sundowns in the first round of the Telkom Knockout. He resigned on Monday last week.
Maritzburg's chairman Farook Kadodia welcomed his new coach at a press conference, saying they were excited to hire what he termed a "young and progressive coach". "Clinton is renowned for his superb man management skills and his dynamic approach to the game and his influence in implementing a more attacking style of football."
No details of the new coach's contract terms were revealed, but Larsen responded: "I will strive to fulfil all the goals of the club. There is a lot of hard work but we are going to work towards our goals together and are confident that we will achieve success."
It has also been confirmed that Maritzburg are to receive a compensation fee from Celtic to buy Middendorp out of his contract.
Kadodia made a formal response to Middendorp's departure on the club's website: "... I am really disappointed [Middendorp was allegedly in talks with Celtic before his resignation] with [his] behaviour as this [is] not what is expected of a head coach."
Larsen and Middendorp are scheduled to go head-to- head when Celtic host Maritzburg at the Free State Stadium on Tuesday, November 5.