Carbon nanotubes with multi-layer graphene sheets (excellent mechanical properties, chemical stability, electrical properties, and thermal properties) are excellent modifiers and ideal functional enhancement materials for composite materials. It has strong adhesion and good overall mechanical properties, but epoxy resin cross-linked and cured after brittle, impact resistance and resistance, stress cracking ability is poor. Therefore, the introduction of nanoparticles in epoxy resin for modification is proved to be a very effective method. This article proposes the modification of carbon nanotubes and graphene sheets, and adds epoxy resin with the help of solution mixing and melt, mixed methods to prepare composite materials. The characterization methods and the modification effects are characterized. Through the mechanical properties, thermal conductivity, and conductivity and electrical properties of the composites, the modification enhancement effect was evaluated, and the mechanism of modification of the impurities is enhanced.