Vandenbroeck, 41, won the three titles including the Tanzania Premier League since replacing compatriot Patrick Aussems at the helm but has now opted to leave the club.
With the 21-time league champions currently nine points behind rivals Young Africans SC, albeit with three games in hand, the Champions League progression has seemingly not appeased the club's demanding hierarchy.
"The Board of Directors of Simba Sports Club announces to its members and fans that we have parted ways with our head coach Sven Vandenbroeck by mutual consent," the club statement read.
"Simba Sports Club thank coach Sven for the success achieved during his time with the club where we won the Tanzanian Premier League, the FA Cup, the Community Shield and qualified for the group stage of the Caf Champions League."
Assistant coach Selemani Matola has taken charge of an interim basis for Wekundu wa Msimbazi as they now look to bridge the gap with Yanga in the league and await their Champions League draw fate.
The former Zambia coach was part of Cameroon's triumphant 2017 Africa Cup of Nations squad as the assistant to Hugo Broos.