The 31-year-old was fast approaching the final six months of his contract with Cape Town City, who announced his departure from the club on Wednesday.
Majoro, an experienced marksman with 10 international caps under his belt, will look to hit the ground running at the Braamfontein-based club in order to help them move away from the relegation zone.
Going into the start of the second half of the campaign, Gavin Hunt's men find themselves rooted at the bottom of the PSL log with 11 points.
His contract with the Students will commence on January 1, 2018, the defending PSL champions announced.
Bidvest Wits is pleased to announce the signing of Lehlohonolo Majoro with effect from 1 January 2018. Welcome to the Clever Boys family. #nakanjani
— Bidvest Wits (@BidvestWits) December 27, 2017
Majoro scored 11 goals in over 40 appearances for the Citizens during his one-and-a-half-year stint in the Mother City.
He was recently linked with a possible move to SuperSport United, but indications were there that he would be heading to Braamfontein.
Major, as he's affectionately known, made a name for himself at AmaZulu before joining Amakhosi in 2011.
He moved to Bucs in 2013 after deciding against renewing his contract with them, but he could only manage 46 appearances in all competitions during his three-year spell at the Sea Robbers.