The utilization of sheet structure composites as a viable conductive filler has been implemented in polymer-based electromagnetic shielding materials. However, the development of an innovative sheet structure to enhance electromagnetic shielding performance remains a significant challenge. Herein, we propose a novel design incorporating silver-modified nanosheet self-assembled hollow spheres to optimize their performance. The unique microporous structure of the hollow composite, combined with the self-assembled surface nanosheets, facilitates multiple reflections of electromagnetic waves, thereby enhancing the dissipation of electromagnetic energy. The contribution of absorbing and reflecting electromagnetic waves in hollow nanostructures could be attributed to both the inner and outer surfaces. When multiple reflection attenuation is implemented, the self-assembled stack structure of nanosheets outside the composite material significantly enhances the occurrence of multiple reflections, thereby effectively improving its shielding performance. The structure also facilitates multiple reflections of incoming electromagnetic waves at the internal and external interfaces of the material, thereby enhancing the shielding efficiency. Simultaneously, the incorporation of silver particles can enhance conductivity and further augment the shielding properties. Finally, the optimized Ag/NiSi-Ni nanocomposites can demonstrate superior initial permeability (2.1 × 10-6 H m-1), saturation magnetization (13.2 emu g-1), and conductivity (1.2 × 10-3 Ω•m). This work could offer insights for structural design of conductive fillers with improved electromagnetic shielding performance.
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