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In this work, a new compound, N-TMSPrVaC, was synthesized using 3-aminopropyltrimethoxysilane (ATPMS) and valeryl chloride (C5H9ClO). Furthermore, it was grafted onto the silicone polymer (PSOL) to obtain a new epoxy resin modifier. Infrared spectroscopy (FT-IR) and nuclear magnetic resonance spectroscopy (1H NMR) were used to characterize the composition and structure of the compound N-TMSPrVaC. The mechanical properties and dynamic thermomechanical analysis (DMA) of PSOL-(N-TMSPrVaC)/EP composites were systematically studied. PSOL-(N-TMSPrVaC) can significantly improve the tensile properties and impact properties of composites by 8.9% (0.5 phr) and 18.2% (3.0 phr), respectively, according to the results. The distribution of PSOL-(N-TMSPrVaC) in the epoxy was studied using the scanning electron microscope and X-ray spectrometry (SEM-EDS). The DMA test showed that the functionalized silicon polymer retained the heat resistance of the epoxy composite material to a certain extent while toughened the epoxy.