The rapid growth of electronic communications has intensified electromagnetic pollution, creating an urgent need for lightweight, high-performance electromagnetic interference (EMI) shielding materials. Carbon fiber reinforced polymer composites (CFRPs) are attractive candidates due to their high specific strength, stiffness, and design flexibility, but their practical application is limited by inherently weak fiber-matrix interfaces and electrical conductivity significantly lower than metals. Inspired by the strong, versatile adhesion of mussels, we developed a hybrid coating on carbon fiber through sequential deposition of Fe3+-tannic acid metal-phenolic networks (MPNs), followed by in situ growth of silver nanoparticles (Ag NPs) via catechol-mediated reduction. This MPN-Ag hybrid network effectively enhances both interfacial mechanics and electrical properties. Mechanically, the smooth modulus gradient created by the hybrid interphase improves stress transfer and promotes cohesive resin failure, resulting in remarkable enhancements in interfacial property, with interfacial shear strength and transverse fiber bundle strength increasing by 85 % and 67 %, respectively. Moreover, the conductive MPN-Ag layer facilitates multiple EMI attenuation mechanisms, including reflection, conduction, and interfacial polarization losses, achieving an outstanding EMI shielding effectiveness of 22.7 dB at just 1 mm thickness. This facile, scalable strategy integrates structural reinforcement with functional performance, offering a pathway to multifunctional CFRPs capable of simultaneous mechanical robustness and effective EMI shielding. Such an approach advances the development of next-generation CFRPs for aerospace, electronics, and other advanced structural-functional applications, bridging the gap between high-performance composites and emerging multifunctional material demands.
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