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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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