Silica aerogels are attractive materials for various applications due to their exceptional performances and open porous structure. Especially in thermal management, silica aerogels with low thermal conductivity need to be processed into customized structures and shapes for accurate installation on protected parts, which plays an important role in high-efficiency insulation. However, traditional subtractive manufacturing of silica aerogels with complex geometric architectures and high-precision shapes has remained challenging since the intrinsic ceramic brittleness of silica aerogels. Comparatively, additive manufacturing (3D printing) provides an alternative route to obtain custom-designed silica aerogels. Herein, we demonstrate a thermal-solidifying 3D printing strategy to fabricate silica aerogels with complex architectures via directly writing a temperature-induced solidifiable silica ink in an ambient environment. The solidification of silica inks is facilely realized, coupling with the continuous ammonia catalysis by the thermolysis of urea. Based on our proposed thermal-solidifying 3D printing strategy, printed objects show excellent shape retention and have a capacity to subsequently undergo the processes of in situ hydrophobic modification, solvent replacement, and supercritical drying. 3D-printed silica aerogels with hydrophobic modification show a super-high water contact angle of 157°. Benefiting from the low density (0.25 g·cm^-3) and mesoporous silica network, optimized 3D-printed specimens with a high specific surface area of 272 m²·g^-1 possess a low thermal conductivity of 32.43 mW·m^-1·K^-1. These outstanding performances of 3D-printed silica aerogels are comparable to those of traditional aerogels. More importantly, the thermal-solidifying 3D printing strategy brings hope to the custom design and industrial production of silica aerogel insulation materials.

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