Graphene nanowalls (GNWs) with different sizes (i.e., length and height) were grown directly on the surface of individual carbon fibers (CFs) using a radio frequency plasma-enhanced chemical vapor deposition (RF-PECVD) technique. The size was controlled by varying the deposition time. The GNW-modified CFs were embedded into epoxy resin matrix to prepare a series of carbon-fiber-reinforced composites (CFRCs). The results indicated that GNWs were remarkably effective in improving the interfacial shear strength (IFSS) and interlaminar shear strength (ILSS) of the carbon-fiber-reinforced composites. The enhancement effect on the strength strongly depended on the size of GNWs. It increased with the increase in the GNWs’ size and reached the maximum upon the incorporation of GNWs that were grown for 45 min. Noticeable increases of 222.8% and 41.1% were observed in IFSS and ILSS, respectively. The enhancement mechanism was revealed by means of scanning electron microscope (SEM) fractography analysis. However, further increase of GNW size led to no more improvement in the shear strength. It could result from the increased defect concentration and wrinkle size in the GNWs, which deteriorated the strength.