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Carbon nanofibers are promising as primary electrode materials for supercapacitors on account of high specific surface area, lightweight, superior physicochemical stability, rich resource, and renewability. However, constructing porous and flexible carbon electrode materials with high capacitance for practical applications remains challenging. Here, heteroatom-decorated hierarchical porous carbon nanofiber composites containing phosphazene [N 3 P 3 (p-OC 6 H 4 -p-CHO) 6 , HAPCP], polymethyl methacrylate (PMMA), and graphene oxide (GO) are prepared through one-step electrospinning and subsequent thermal treatment. The alternant phosphorus−nitrogen structure links to the carbon backbones to improve flexibility and electrochemical performance. Inspired by a biomimetic Setaria viridis-like structure, the polyaniline (PANI)-decorated porous hybrid electrodes are prepared. The PANI@GO/PMMA/ HAPCP/PAN carbon nanofibers (400P@0.1GPHCNFs) covered by PANI nanofibers as a novel free-standing flexible electrode exhibit an excellent electrochemical performance of 680.8 F g −1 at 0.5 A g −1 with a good capacitance retention of 93.5% after 3000 cycles. Moreover, the symmetric flexible all-solid-state supercapacitor assembled by the novel and delicate electrodes exhibits a high energy density of 27.70 W h kg −1 (at a power density of 231.08 W kg −1 ) and favorable cycling stability (84.50% retention of the capacitance after 1000 charge−discharge cycles), which indicates that the 400P@0.1GPHCNFs have great potential as a high-performance flexible supercapacitor electrode.

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Lightweight and compressible aerogels have been widely considered as promising materials for electromagnetic interference (EMI) shielding. Herein, a lightweight cellulose nanofibril/reduced graphene oxide carbon aerogel fabricated by unidirectional freeze‐drying and pyrolysis processes is reported. The results show that the aerogels with unidirectionally aligned pores possess better compression resilience and EMI shielding performance in the radial direction. The unidirectional aerogel with low density (≈0.0058 g cm−3) exhibits a high EMI shielding effectiveness (SE) of ≈33 dB at 8.2–12.4 GHz and a specific EMI SE of 5759 dB cm3 g−1. Therefore, the fabricated aerogel demonstrates a promising potential in the field of next‐generation EMI shielding materials.

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