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The structural integrity and continuity are prerequisites for exploiting the performance advantages of aerogels, while limitations in mechanical properties, such as low strength, high brittleness, and poor processability confine fully intact aerogels to laboratory settings. Here, a composite aerogel SPCCAM designed with hierarchical structuring into 1D building blocks at the nanoscale and honeycomb‐like anisotropic architecture at the microscale is presented. The inner carboxylated cellulose nanofiber core (CNFs‐C) exhibits much higher strength than the intermediate polybenzoxazine (PBOZ) shell, and the interface is highly reinforced by a crosslinked network of amino and hydrogen bonds, forming a highly stable 1D building block. Superhydrophobic SiO2 nanoparticle (hydrophobic‐260) is discretely distributed on the outer surface of the PBOZ shell, resulting in a nanoscale lotus leaf effect. Thus, the SPCCAM demonstrates outstanding properties including ultrahigh strength, excellent deformability and fatigue resistance, good machinability, ultralow thermal conductivity and coefficient of linear expansion, and superhydrophobicity from the inside out and long‐term hydrophobic stability along the radial direction of microscale channels, defining a novel method for designing aerogels with superior integrated mechanical, thermal insulation, and hydrophobic properties, and offering an attractive solution for high‐efficiency thermal insulators in high‐moisture extreme environments, such as deep‐sea and polar regions. [ABSTRACT FROM AUTHOR]

The development of Li-free anodes to inhibit Li dendrite formation and provide high energy density Li batteries is highly applauded. However, the lithiophobic interphase and heterogeneous Li deposition hindered the practical application. In this work, a 20 nm ultra-sleek high entropy alloy (HEA, NiCdCuInZn) tights loaded with HEA nanoparticles are developed by a thermodynamically driven phase transition method on the carbon fiber (HEA/C). Multiple Li + transport paths and abundant active sites are enabled by the cocktail effect of different constituent elements in HEA. These active sites with gradient absorption energies (-3.18 to -2.03 eV) facilitate selective binding, providing a low barrier for homogeneous Li nucleation. Simultaneously, multiple transport paths promote Li diffusion behavior with uniform Li deposition. Thus, the HEA/C achieves high reversibility of Li plating/stripping processes over 2000 cycles with a coulombic efficiency of 99.6% at 5 mA cm -2 /1 mAh cm -2 in asymmetric cells, as well as over 7200 h at 60 mA cm -2 /60 mAh cm -2 in symmetric cells. Moreover, the anode-free full cell with the HEA/C host has an average coulombic efficiency of 99.5% at 1 C after 160 cycles. This advanced HEA structure design shows a favorable potential application for anode-free Li metal batteries., (© 2023 Wiley-VCH GmbH.)