In the microelectronics era, electromagnetic radiation and heat accumulation in electronic devices are urgent challenges requiring solutions, particularly through the use of structure-function integrated and lightweight materials for electromagnetic interference (EMI) shielding and thermal management. Hierarchically structured polyether-ether-ketone-based composites are prepared in this study by in situ deposition and dip coating using a simple and scalable method. Magnetic cobalt nanoparticles derived from magnetic metal-organic frameworks are deposited on carbon fiber felt featuring a macroscopic continuous conductive network. Next, a hybrid slurry is applied to connect the isolated fibers, which bridge the fiber gaps to create new electron and phonon transport channels, increasing the thermal conductivity (23.43 Wm-1K-1 in plane, 4.84 Wm-1K-1 through plane) for efficient heat dissipation. Owing to the stable 3D crosslinked network with high electrical conductivity (13608 Sm-1), the composite offers ultra-high EMI shielding in the X-band (101.64dB with stability in extreme environments), excellent Joule heating performance (220°C at 4V), and excellent photothermal conversion (94°C at 500 mWcm-2). This multifunctional composite material has great application prospects in precision electronic equipment.
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