In this work, inspired by the great advantage of the unique “brick‐mortar” layered structure as electromagnetic interference (EMI) shielding materials, a multifunctional flexible graphene nanosheets (GNS)/polytetrafluoroethylene (PTFE) composite film with excellent EMI shielding effects, impressive Joule heating performance, and light‐to‐heat conversion efficiency is fabricated based on the self‐emulsifying process of PTFE. Both PTFE microspheres and nanofibers are employed together for the first time as “sand and cement” to build unique nacre‐structured EMI shielding materials. Such configuration can obviously enhance the adhesion of composites and improve their mechanical property for the application under extreme environment. Moreover, the simple and effective repetitive roll pressing method can be used for the scalable production in industrialization. The GNS/PTFE composite film shows a high EMI shielding effectiveness (SE) of 50.85 dB. Furthermore, it has a high thermal conductivity of 16.54 W (m K)−1, good flexibility, and recyclable properties. The excellent fire‐resistant and hydrophobic properties of GNS/PTFE film also ensure its reliability and safety in practical application. In conclusion, the GNS/PTFE film demonstrates the potential for industrial manufacturing, and outstanding EMI shielding performance with high stability and durability, which has a broad application prospect for electronic devices in practical extreme outdoor environments.

With the explosive development of modern military detection technology, stealth compatibility for materials with both outstanding microwave absorption (MA) and low infrared emissivity is urgently needed. In this paper, indium...

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