In this study, CNTs were grafted onto carbon fibers using Ni deposited film as the catalyst, and their interfacial properties were evaluated for the purpose of figure out the significant effect of CNTs introduced at the fiber/resin interface in CFRP laminates. CNTs were grafted onto carbon fiber surfaces without any significant degradation of tensile properties. CNT-grafted fibers also showed the remarkable interfacial and interlaminar properties. Interfacial shear strength of CNT-grafted fibers indicated 224% improvement compared with as-received ones. Furthermore, hierarchical CFRP laminate was fabricated and intelaminar shear strength was studied. As a result, interlaminar shear strength has increased by 32%. Those beneficial results derive from an anchor effect of CNTs introduced to the fiber/resin interfaces.