SiC/EP composites are promising insulating materials due to their high thermal conductivity, stable chemical properties, and nonlinear electrical conductivity. However, the compatibility of micron-sized SiC particles with the organic polymer matrix is poor, and defects such as air gaps may be introduced at the interface, which reduces the partial discharge resistance of the composite materials. In order to improve the partial discharge initial voltage (PDIV) of SiC/EP composites, in this paper, SiC/EP composites with different proportions were prepared by surface modification of filler and compound of micro/nano particles. Firstly, a method of secondary modification of SiC particles was proposed, which was first modified by alkali washing and then silane coupling agent KH560, and the effectiveness of the modification was verified. Therefore, the interface bonding ability between the filler and the matrix was improved, the air gap defects at the interface were reduced, and the PDIV of the composite material was improved. When the filling ratio is 10 wt%, the PDIV was enhanced by 13.75%, and when the filling ratio was further increased, the improvement was reduced. In contrast, the introduction of nanoparticles into the composites can effectively improve the PDIV of composite materials. In this study, nanoparticles were used to form a shell-core structure in epoxy resins to exert their huge specific surface area and active surface properties, thereby changing the overall crosslinking properties of the composites. Through experimental research, the optimal micro-nano particle compounding ratio was explored. Under the optimal mixing ratio, the PDIV of the composite material can be increased by more than 90%.