| Summary: | This paper proposes dual-functional sheets (DFSs) that simultaneously have high thermal conductivity (TC) and electromagnetic interference (EMI) absorbing properties, making them suitable for use in mobile electronics. By adopting a simple but highly efficient dry process for manufacturing core–shell structured fillers (CSSFs) and formulating a close-packed filler composition, the DFSs show high performance, TC of 5.1 W m<sup>−1</sup> K<sup>−1</sup>, and a −4 dB inter-decoupling ratio (IDR) at a 1 GHz frequency. Especially, the DFSs show a high dielectric breakdown voltage (BDV) of 3 kV mm<sup>−1</sup>, which is beneficial for application in most electronic devices. The DFSs consist of two kinds of CSSFs that are blended in accordance with the close-packing rule, Horsfield’s packing model, and with polydimethylsiloxane (PDMS) polymers. The core materials are soft magnetic Fe-12.5%Cr and Fe-6.5%Si alloy powders of different sizes, and Al<sub>2</sub>O<sub>3</sub> ceramic powders of a 1-μm diameter are used as the shell material. The high performance of the DFS is supposed to originate from the thick and stable shell layer and the maximized filler loading capability owing to the close-packed structure.
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