 This study presents the design and fabrication of lightweight nanostructured aerogels for high-performance electromagnetic interference, EMI, shielding using ultra-thin cellulose nanofibrils, CNFs. The resulting emzene-slash-CNF aerogels exhibit ultra-high EMI shielding performance, with an EMI shielding effectiveness of 74.6 or 35.5 dB at a density of 8.0 or 1.5 mg backslash-XA0 CM3, respectively. The normalized surface-specific SE is up to 189 backslash-XA0400 dB backslash-XA0 CM2 backslash-XA0 G1, significantly exceeding that of other EMI shielding materials reported so far. The study reveals the influence of the angles between oriented cell walls and the incident EM wave electric field direction on the EMI shielding performance, providing an intriguing microstructure design strategy. This article was authored by Zhou Huizeng, Zhang Xianwang, Gilberto Sikera, and others. We are article.tv, links in the description below.