Solubility‐pKa Coupling Effect Tailored Nanoporous Nylon Aerogel Family with Multiple Thermomechanical Processes

Abstract Despite significant advancements in aerogels science, the fabrication of high‐performance aerogels with their plastic processability remains unexplored owing to their inherent trade‐off between skeletal rigidity and transformable processability. Herein, a universal solubility‐pKa coupling‐effect to engineer high‐performance thermoplastic nylon aerogel family with excellent thermomechanical processing performance is proposed. By modulating solubility parameters and acid dissociation constants in nylon‐solvent systems, it is precisely control crystallization to assemble interlaced 1D nanofiber skeletons, yielding nylon aerogels that integrate a high specific surface area (226 m 2 g −1 ), exceptional compressive modulus (12.6 MPa), and ultralow thermal conductivity (0.034 W m −1 K −1 ). Notably, beyond achieving performance comparable to aramid and other high‐performance aerogels, these nylon aerogels uniquely incorporate thermoplastic properties enabling multiple thermomechanical processing for aerogel functionalization, including protective barrier via thermal encapsulating, reassembly of aerogel unmanned aerial vehicle through thermal cutting and welding, and biomimetic hydrophobic surfaces with lotus and petal effects through precise thermal imprinting. Surprisingly, thermomechanical processing also induces fluorescence of aerogels, suggesting applications in thermal‐recording, anti‐counterfeiting, etc. This research overcomes the critical skeletal rigidity‐transformable processability trade‐off in aerogels, enabling novel manufacturing approaches and broader engineering applications.