The electromagnetic interference (EMI) shielding performance of reduced graphene oxide (rGO) foam is restricted to its poor conductivity and macro‐monotonic structure. In this work, highly conductive MXene nanosheets are introduced into graphene oxide (GO) solution and multilayer structures were designed to improve the EMI shielding performance of graphene foam. The multilayer rGO/MXene composite foam shows an excellent EMI shielding effectiveness of more than ≈28 dB in C and ≈35 dB in X band. Meanwhile, it reveals an outstanding heat insulation performance equaling to air (0.025 W m−1 K). The macro multilayer and microporous structure plays a prominent role in the EMI shielding and heat insulation performance. This work provides valuable ideas for designing multifunctional EMI shielding materials for the next generation of smart electronic devices.
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