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Surface modification is a fascinating way to improve the compounding effect between inorganic fillers and polymers. In this study, zirconium tungsten phosphate (ZWP) with negative thermal expansion was surface modified by silane coupling agent 3-(Trimethoxysilyl)propyl methacrylate. The effects of surface modification and the modification mechanism were analyzed in detail by X-ray diffractometer, scanning electron microscopy, Fourier transform infrared spectroscopy and thermal mechanical analysis. The surface modification could effectively reduce the thermal expansion properties of the composite. When the added amount of 3-methacryloxypropyl trimethoxysilaneSilane (trade name: KH570) is 0.50 wt%, the thermal expansion coefficient of ZWP/Aromatic polyimide composite decreased by 9.76%. The surface modification also can effectively improve the dielectric performance of aromatic polyimides. The present work provides one new way to improve the thermal expansion behavior of composites.