The Belgian Football Association announced on Monday that it had decided not to extend the 62-year-old Frenchman's deal, bringing his 18-month spell in charge to an end.
Garcia guided Belgium to the quarter-finals of this month's FIFA World Cup, where they were beaten by eventual champions Spain. Despite that run, questions remained over the team's overall performances during the tournament, with their displays failing to fully convince.
Belgium's sporting director Vincent Mannaert thanked Garcia for his work and said the coach had helped steady the national team during a difficult period.
"Rudi Garcia has unquestionably played a key role in restoring the Belgian Red Devils," Mannaert said.
"He was appointed national coach in a challenging sporting and financial context. Thanks in particular to his commitment and experience, team cohesion was restored and a strong result was achieved at the most recent World Cup."
Mannaert also paid tribute to Garcia and his coaching staff before confirming the search for a successor is already underway.
"On behalf of the federation, I would like to warmly thank Rudi and his assistants for the past 18 months," he said.
"Together with my team, I am currently preparing for a new cycle, including the appointment of a new national coach."