In the present research, to enhance interfacial wettability and adhesion between carbon fibers (CFs) and matrix resin, hydrophilic silica nanoparticles (SiO2) were utilized to graft the surface of CFs. Polydopamine (PDA) as a âbio-glueâ was architecturally built between SiO2 and CFs to obtain a strong adhesion strength and homogenous SiO2 distribution onto the surface of CFs. The facile modification strategy was designed by self-polymerization of dopamine followed by the hydrolysis of tetraethoxysilane (TEOS) onto carbon fibers. Surface microstructures and interfacial properties of CFs, before and after modification, were systematically investigated. The tight and homogeneous coverage of SiO2 layers onto the CF surface, with the assistance of a PDA layer by self-polymerization of dopamine, significantly enhanced fiber surface roughness and wettability, resulting in an obvious improvement of mechanical interlocking and interfacial interactions between CFs and matrix resin. The interlaminar shear strength (ILSS) and the interfacial shear strength (IFSS) of CF/PDA/SiO2 reinforced composites exhibited 57.28% and 41.84% enhancements compared with those of untreated composites. In addition, impact strength and the hydrothermal aging resistance of the resulting composites showed great improvements after modification. The possible reinforcing mechanisms during the modification process have been discussed. This novel strategy of developed SiO2-modified CFs has interesting potential for interfacial improvements for advanced polymer composites.