ITQ-37 and ITQ-43 possessing mesoporous structures have aroused great interest because of their promising applications involving large molecules. However, it is challenging to synthesize these zeolites. Herein, MAS-ITQ-37 and MAS-ITQ-43 with enhanced Si/Ge ratios of 1.7 and 3.0 have been synthesized by using a simple matrine-derived organic structure-directing agent.