Based on the fact that C60 is one of the most abundant and readily available molecular configurations in the fullerene family, this paper investigates the effect of doping fullerenes on the dielectric properties of epoxy composites using C60 as a representative. The structure and properties of fullerene molecules are thoroughly examined from the point of view of materials chemistry. The equipment required for the experiment is selected, the experimental sample preparation plan is formulated, and the structure and dielectric properties of the prepared samples are analyzed by corresponding data analysis. The results show that in the range of r less than 1.03 Å, the particle distribution probability of the fullerene-doped epoxy composites in this interval is 0. As r continues to increase, the probability density of the fused C60 epoxy composites is higher than that of the epoxy matrix. The frequency band of 1 MHz has an enhancement of 0.053 and 0.043. However, the dielectric constant of the composite epoxy resin in the high-frequency interval gradually falls back with the increase of filler, while the enhancement of the dielectric constant occurs in the low-frequency interval, and the fullerene is also optimized in terms of the dielectric constant and dielectric loss properties. Fullerene’s excellent dielectric properties have been confirmed by this study, which is important to broaden the epoxy resin market and improve the competitiveness of products.