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To improve the accessibility of polyimide aerogels (PAs) in diverse application scenarios, the major objective is to create PAs in dimension/geometry on demand. However, their ability to deliver excellent performance and expanded applications remains challenging. Herein, the three-dimensional (3D) printing of Pas, which simultaneously addresses the above concerns, is proposed using a combination of a one-step chemical-imidization sol–gel strategy and direct ink writing. The resultant 3D-printed PAs exhibit many desirable properties, such as high specific surface area (561.7 m2 g−1), low density (66.1 ± 1.4 kg m−3), low thermal conductivity (39.89 ± 0.16 mW m−1 K−1), low shrinkage (<7%), exceptional thermal stability (up to 450 °C) and good mechanical properties. They also possess excellent heat/cold preservation, heat/cold/moisture insulation, air/light permeability, and ammonia/moisture adsorption. All of these are highly desirable for addressing severe environmental concerns. Moreover, the application scalability of 3D-printed PAs is confirmed by the successful incorporation of carbon nanotubes, and the subsequent expanded functionality and application potential. The flexibility of inks/materials and the manipulability of the structures and functions, demonstrates great prospect for synergy management of thermal insulation, gas permeability and light absorption, thus expanding the application of PAs. [ABSTRACT FROM AUTHOR]