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Aerogels are widely recognized for their extreme porosity, low density, and thermal superinsulation ability, but their inherent fragility has long limited their broader applications. In this work, we demonstrate how precise engineering of both chemical composition and microstructure can overcome these limitations, enabling aerogels with superior mechanical performance while retaining their unique characteristics. Focusing on poly(organosiloxane) (silicone)-based systems, we utilize controlled sol-gel chemistry to produce highly porous, yet mechanically robust aerogels. By optimizing the hydrolysis and polycondensation of methyltrimethoxysilane in the presence of cationic surfactants, we obtain uniform mesoporous networks composed of interconnected colloidal structures, which impart flexibility under compressive loading. This flexibility allows ambient pressure drying, facilitated by reversible shrinkage and spring-back behavior during solvent removal. Moreover, introducing a Pluronic-type block copolymer surfactant directs the growth of fibrous silicone networks at the mesoscale, yielding aerogels with remarkable bending flexibility. This combination of tunable chemical composition and microstructural design offers a powerful route to produce aerogels with exceptional mechanical resilience, expanding their potential for diverse advanced applications.