Syiem was suspended by the Congress last year after he rebelled against Chief Minister Mukul Sangma.
"I hereby tender my resignation of my seat in the House with immediate effect from December 15, 2017," he said in a letter submitted to Speaker A T Mondal.
Syiem said he will join the new political party, the Peoples' Democratic Front (PDF) and will contest the state Assembly elections due early next year on PDF ticket.
Syiem is also the chief executive member of the Khasi Hills Autonomous District Council (KHADC).
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