In this study, nano-scale fillers are added to epoxy matrix-based carbon fibers-reinforced composites (CFRPs) to improve the mechanical properties of multi-scale composites. Single-walled carbon nanotubes (SWCNTs) used as nano-scale fillers are treated with atmospheric-pressure plasma to introduce oxygen functional groups on the fillers’ surface to increase the surface free energy and polar component, which relates to the mechanical properties of multi-scale composites. In addition, the effect of dispersibility was analyzed through the fracture surfaces of multi-scale composites containing atmospheric-pressure plasma-treated SWCNTs (P-SWCNTs) under high load conditions. The fillers content has an optimum weight percent load at 0.5 wt.% and the fracture toughness (KIC) method is used to demonstrate an improvement in mechanical properties. Here, KIC was calculated by three equations based on different models and we analyzed the correlation between mechanical properties and surface treatment. Compared to the composites of untreated SWCNTs, the KIC value is improved by 23.7%, suggesting improved mechanical properties by introducing selective functional groups through surface control technology to improve interfacial interactions within multi-scale composites.