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The hydrophobic nature of inorganic zeolite particles plays a crucial role in the efficacy of mixed matrix membranes (MMMs) for the separation of trichloroethylene (TCE) through pervaporation. This study presents a novel approach to further augment the hydrophobicity of ZSM-5. The ZSM-5 zeolite molecular sieve was subjected to modification using three different silane coupling agents, namely, n-octyltriethoxysilane (OTES), γ-methacryloxypropyltrimethoxysilane (KH-570), and γ-aminopropyltriethoxysilane (KH-550). The water contact angles of the resulting OTES@ZSM-5, KH-570@ZSM-5, and KH-550@ZSM-5 particles exhibited significant increases from 97.2° to 112.8°, 109.1°, and 102.7°, respectively, thereby indicating a notable enhancement in hydrophobicity. Subsequently, mixed matrix membranes (MMMs) were fabricated by incorporating the aforementioned silane-modified ZSM-5 particles into polydimethylsiloxane (PDMS), leading to a considerable improvement in the adsorption selectivity of these membranes towards trichloroethylene (TCE). The findings indicate that the PDMS membrane with a 20 wt.% OTES@ZSM-5 particle loading exhibits superior pervaporation performance. When subjected to a temperature of 30 °C, flow rate of 100 mL/min, and vacuum of 30 Kpa, the separation factor and total flux of a 3 × 10⁻⁷ wt.% TCE solution reach 328 and 155 gm⁻²·h⁻¹, respectively. In comparison to the unmodified ZSM-5/PDMS membrane, the separation factor demonstrates a 41% increase, while the TCE flux experiences a 6% increase. Consequently, this approach effectively enhances the pervaporation separation capabilities of the PDMS membrane for TCE.