The problem of interfacial interaction between carbon fiber (CF) and the matrix is the key to the failure of CF-reinforced plastic (CFRP). A general strategy to enhance interfacial connections is to create covalent bonds between the components, but this usually reduces the toughness of the composite material, which in turn limits the range of applications of the composite. In this study, carbon nanotubes (CNTs) were grafted onto the CF surface using the molecular layer bridging effect of the dual coupling agent to prepare multi-scale reinforcements, which significantly improved the roughness and chemical activity of the CF surface. By introducing a transition layer structure between the carbon fibers and the epoxy resin matrix to moderate the large modulus and scale differences between them, the interfacial interaction was improved while enhancing the strength and toughness of CFRP. We used amine-cured bisphenol A-based epoxy resin (E44) as the matrix resin and prepared the composites by the hand-paste method and performed tensile tests on the prepared composites, which showed that, compared with the original CF-reinforced composites, the modified composites showed an increase in tensile strength, Young’s modulus and elongation at break by 40.5%, 66.3% and 41.9%, respectively.