A 3D-printing process is presented for the manufacturing of modular aerogel/acrylate bricks that are fully scalable and customizable for potential applications in thermal insulation. The use of 3D-printing tools in conjunction with a sol-gel method of aerogel synthesis circumvents the geometric limitations of fabrication of large size load bearing aerogel articles. In this study, two-component aerogel bricks are manufactured from the low thermal conductivity of aerogels and 3D-printed load-bearing polymer bricks. For this purpose, aerogels are synthesized from polyimide and partially crosslinked stereolithography acrylate (SLA) resins. The aerogel materials are held by mechanically strong LEGO®-like bricks derived from fully crosslinked SLA resin and fully cured epoxy resin. The transient temperature profiles on brick surfaces due to contact heating and flexural and compressive properties of bricks filled with aerogel materials are discussed.