Aerogels were listed among the top ten emerging technologies in chemistry by IUPAC in 2022. Their record-breaking properties sparked the emergence of a thriving insulation market, but solutions are sought to promote additional applications. A 3D assembly process based on direct ink writing of "aerogel-in-aerogel" nanocomposites is presented. The printed polyimide-silica aerogels are non-brittle (E = 6.7 MPa) with a super-insulating thermal conductivity (20.3 mW m⁻¹ K⁻¹) and high thermal stability (T_5wt% 447 °C). In addition, they display excellent low-loss dielectric properties and microwave transmission over all relevant communication bands and can be functionalized for electromagnetic interference (EMI) shielding. The high shape-fidelity printing, combined with laser-induced etching of thermally conductive graphene layers, enable precise thermal management for portable electronics or maintain an extreme temperature gradient (−40 to +50°C) across a millimeter-scale partition.