Multiscale hybrid composites, which consist of polymeric resins, microscale fibers and nanoscale reinforcements, have drawn significant attention in the field of advanced, high-performance materials. Despite their advantages, multiscale hybrid composites show challenges associated with nanomaterial dispersion, viscosity, interfacial bonding and load transfer, and orientation control. In this paper, carbon nanotube(CNT)/carbon fiber(CF)/ polycarbonate(PC) multiscale hybrid composite were fabricated by a solution process to overcome the difficulties associated with controlling the melt viscosity of thermoplastic resins. The dependence of CNT loading was studied by varying the method to add CNTs, i.e., impregnation of CF with CNT/PC/solvent solution and impregnation of CNTcoated CF with PC/solvent solution. In addition, hybrid composites were fabricated through surfactant-aided CNT dispersion followed by vacuum filtration. The morphologies of the surfaces of hybrid composites, as analyzed by scanning electron microscopy, revealed the quality of PC impregnation depends on the processing method. Dynamic mechanical analysis was performed to evaluate their mechanical performance. It was analyzed that if the position of the value of tan δ is closer to the ideal line, the adhesion between polymer and carbon fiber is stronger. The effect of mechanical interlocking has a great influence on the dynamic mechanical properties of the composites with CNTcoated CF, which indicates that coating CF with CNTs is a suitable method to fabricate CNT/CF/PC hybrid composites.