In this article, chlorosilane-modified ZSM-5 particles were incorporated into polydimethylsiloxane (PDMS) to form mixed matrix membranes (MMMs) for ethanol/ water mixture separation via pervaporation (PV). The membranes were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, and mechanical performance testing. The maximum loading and dispersion of ZSM-5 into PDMS were improved by chlorosilane modification. To evaluate the PV performance, the MMMs were used to separate an aqueous ethanol solution. The effect of zeolite loading and operational conditions on PV performance was investigated in detail. The separation factor of the composite membranes filled with modified ZSM-5 increased considerably versus unmodified membrane, while the total flux decreased to some degree. Of all the chlorosilane-modified membranes, dodecyltrichlorosilane modified ZSM-5 filled PDMS showed the best separation factor of 15.8 for ethanol. POLYM. COM-POS., 37:1282-1291