With the development of the integrated circuit and chip industry, electronic products and their components are becoming increasingly miniaturized, high-frequency, and low-loss. These demand higher requirements for the dielectric properties and other aspects of epoxy resins to develop a novel epoxy resin system that meets the needs of current development. This paper employs ethyl phenylacetate cured dicyclopentadiene phenol (DCPD) epoxy resin as the matrix and incorporates KH550 coupling-agent-treated SiO2hollow glass microspheres to produce composite materials with low dielectric, high heat resistance, and high modulus. These materials are applied as insulation films for high density interconnect (HDI) and substrate-like printed circuit board (SLP) boards. The Fourier transform infrared spectroscopy (FTIR) technique was used to characterize the reaction between the coupling agent and HGM, as well as the curing reaction between the epoxy resin and ethyl phenylacetate. The curing process of the DCPD epoxy resin system was determined using differential scanning calorimetry (DSC). The various properties of the composite material with different HGM contents were tested, and the mechanism of the impact of HGM on the properties of the composite material was discussed. The results indicate that the prepared epoxy resin composite material exhibits good comprehensive performance when the HGM content is 10 wt.%. The dielectric constant at 10 MHz is 2.39, with a dielectric loss of 0.018. The thermal conductivity is 0.1872 Wm−1k−1, the coefficient of thermal expansion is 64.31 ppm/K, the glass transition temperature is 172 °C, and the elastic modulus is 1221.13 MPa.