Biomineralization‐inspired growth of different microstructure <scp>layer double hydroxides</scp> for improving mechanical and tribological properties of carbon fiber/phenolic composites

Abstract Multiscale reinforcements containing controllable inorganic nanomaterials are one of the effective strategies to construct carbon fibers/phenolic resin composites (CFRCs) with a higher load‐bearing interface. Inspired by biomineralization, a series of biomimetic‐structural layer double hydroxides (LDHs) nanomaterials were efficiently grown onto the carboxyl‐grafted carbon fibers (CFs) by precisely adjusting the content of methacrylic acid (MAA) via Diels–Alder chemistry, forming shapes ranging from bromeliad‐like to honeycomb‐like to scale‐like Optimal performances of the CFs‐MAA‐LDHs/phenolic composites are achieved with a honeycomb‐like LDHs structure, among which the tensile strength and flexural strength increased to 572.5 and 220.7 MPa, showing an improvement of 41.7% and 57.1%, respectively. The vertically interweaved distribution of LDHs on the CF surface induces a synergistic effect of mechanical interlocking‐chemical interaction‐wettability‐curing properties. In addition, the wear rate of modified composites was as low as 3.128 × 10 −14 m 3 (Nm) −1 under reciprocating sliding friction, exhibiting a 119.7% increase in wear resistance. It was attributed to the higher reinforcement efficiency and tribological film derived from LDHs nanomaterials. This work provides new insights into the regulation of structural changes of 2D nanomaterials for designing interfacial structures of carbon fiber/phenolic composites. Highlights The carboxylated CFs were prepared by mild and simple Diels–Alder chemistry. A series of biomimetic‐structural LDHs were grown on carboxylated CFs. The physiochemistry–wettability–curing remarkably enhanced the interface. A 41.7% increase in tensile strength and 119.7% increase in wear resistance with LDHs.