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A nanocomposite strategy for the combination of a polymerized silica precursor, such as polyvinyltrimethoxysilane (P-VTMS), together with electrospun thermoplastic polyurethane (TPU) nanofiber in the aerogel backbone is demonstrated to create effective stress transfer pathways in three-dimensional (3-D) aerogel composites with thermal insulation characteristics and special porous structure. Inspired by the bone architecture in the human body, with large amounts of hard segments and small amounts of soft segments, the 3-D interconnected TPU-embedded P-VTMS-based composite (P-VTMS/TPU) aerogel achieves synergistic strengthening in the nanofiber orientation direction. The sol–gel approach followed by first spinodal decomposition and later binodal decomposition phase separation has been taken in this study to initiate network formation throughout the P-VTMS/TPU backbone to form a 3-D network …