Booysen joins the Soweto giants from Ajax Cape Town, signing a two-year deal with an option for a further year.
The 30-year-old becomes Chiefs' second signing of the day, following the arrival of free agent Lebogang Manyama.
“If you set yourself goals you aim for the best and Chiefs are just that,” Booysen told the club's official website.
“It’s been a lifelong aspiration to play for this club as I have always felt that Kaizer Chiefs are far ahead of all other South African clubs. They are true leaders, all others follow.”
Booysen has also featured for Maritzburg United and SuperSport United in the past.