A novel homogeneous floccular chitosan was directly grafted onto carbon fiber surface by a simple and controllable method. Scanning electron microscopy (SEM), single fiber strengths and interlaminar shear strength (ILSS) have been applied to characterize the fiber and the interface bonding. Compared with raw carbon fibers, the chitosan-treated ones demonstrate significant increases in the surface roughness and wettability. Particularly, about 21.21% increase in the mechanical properties of composites was obtained, which is attributed to good adhesion between functional carbon fiber and resin matrix in the interlaminar regions, as revealed by fracture surfaces.