We describe lightweight three-dimensional (3D) graphene hybrid SiO2 aerogels (GSAs) with hierarchically robust interconnected networks fabricated via an in situ deposition procedure after a hydrothermal assembling strategy with graphene oxide sheets. The nano-/micron-thick SiO2 coating conformably grew over porous graphene templates with two constituents (e.g., graphene and SiO2) and formed chemically bonded interfaces. In addition, it significantly refined the primary graphene pores by hundreds of microns into smaller porous patterns. Studies of its mechanical properties verified that the graphene interframework made the ceramic composites elastic, while SiO2 deposition enhanced the strength required it to resist deformation. The higher SiO2 contents resulted in lower elasticity but larger strength because of the apparent nanosize effect of SiO2 ceramic thickness; GSAs with a density of 82.3–250.3 mg/cm3 (corresponding to SiO2 sol with concentration ranging from 5 to 20 wt %) could reach a good balance of strength and elasticity. Benefiting from hierarchical micronetworks consisting of semiclosed or closed pores, GSAs offer excellent thermal-insulation performance, with thermal conductivity as low as 0.026 W/(m·K). GSAs offer improved fire-resistant capacity rather than that of pure carbon-based aerogels via the synergic protection of SiO2 ceramic accretion. This highlights the promising applications of GSAs as lightweight thermal-shielding candidates for industrial equipment, civil architectures, and defense transportation vehicles.
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