Electrostatic adsorption was used to self‐assemble layers of polymers and nanoparticles with varying charges onto the carbon fiber (CF) surface. This process created two distinct ionic crosslinked network layers: (3‐aminopropyl) triethoxysilane‐phytic acid‐polyethyleneimine (APTES‐PA‐PEI) and (3‐aminopropyl) triethoxysilane‐phytic acid‐nano‐silica (APTES‐PA‐SiO2). Fourier transform infrared spectrophotometer (FTIR) and X‐ray photoelectron spectroscopy (XPS) were used to confirm the presence of ionic interactions. The modified carbon fibers (CFs) exhibited increased surface roughness, higher concentration of functional groups, and improved wettability. Compared to untreated CF composites, the interfacial shear strength (IFSS) and the transverse tensile strength test (TFBT) of CF‐APTES‐PA‐PEI/epoxy composites increased by 67.8% and 62%, respectively. In contrast, the IFSS and TFBT of CF‐APTES‐PA‐SiO2/epoxy composites increased by 63.3% and 52.8%, respectively. The observed strengthening is attributed to the combined effects of ionic crosslinked networks, covalent and hydrogen bonding interactions, enhanced wettability, and the relatively roughened fiber surface. The interfacial layer design approach proposed in this study is both straightforward and effective, demonstrating significant potential for functionalizing CFs. This method is expected to be adaptable for other high‐performance fibers.Highlights
The ionic cross‐linked network interface layers were designed.
IFSS and TFBT were significantly improved.
The enhancement mechanism was elaborated.