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The intensification of electromagnetic (EM) pollution and the development of military detection technology have increased the requirements for EM functional materials. In this study, a molybdenum diselenide@reduced graphene oxide (MoSe2@rGO)-assembled architecture is constructed, where the MoSe2 nanosheets grow uniformly on the rGO sheets. By regulating the contributions of conduction genes and polarization genes, adjustable EM functions of MoSe2@rGO hybrids can be achieved. The reflection loss (RL) of the sample can reach −68.7 dB at a thickness of 2.32 mm, and the maximum effective absorption bandwidth can reach 5.04 GHz. When conduction genes dominate, the MoSe2@rGO hybrids exhibit a 98.7% electromagnetic interference (EMI) shielding efficiency. The design of the EM energy conversion device and the results of the radar cross section (RCS) simulation demonstrate the practical application potential of the material. This work provides inspiration for designing multifunctional EM materials.
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