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HighlightsCellulose aerogels were prepared by hydrogen bonding driven self-assembly, gelation and freeze-drying.    The skin-core structure of CCA@rGO aerogels can form a perfect three-dimensional bilayer conductive network.    Outstanding EMI SE (51 dB) is achieved with 3.05 wt% CCA@rGO, which is 3.9 times higher than that of the co-blended composites.Supplementary Information  The online version contains supplementary material available at 10.1007/s40820-021-00624-4.

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Lightweight, Flexible Cellulose-Derived Carbon Aerogel@Reduced Graphene Oxide/PDMS Composites with Outstanding EMI Shielding Performances and Excellent Thermal Conductivities