Here, we present a comprehensive approach for creating robust, elastic, designer Lunar and Martian regolith simulant (LRS and MRS, respectively) architectures using ambient condition, extrusion-based 3D-printing of regolith simulant inks. The LRS and MRS powders are characterized by distinct, highly inhomogeneous morphologies and sizes, where LRS powder particles are highly irregular and jagged and MRS powder particles are rough, but primarily rounded. The inks are synthesized via simple mixing of evaporant, surfactant, and plasticizer solvents, polylactic-co-glycolic acid (30% by solids volume), and regolith simulant powders (70% by solids volume). Both LRS and MRS inks exhibit similar rheological and 3D-printing characteristics, and can be 3D-printed at linear deposition rates of 1–150 mm/s using 300 μm to 1.4 cm-diameter nozzles. The resulting LRS and MRS 3D-printed materials exhibit similar, but distinct internal and external microstructures and material porosity (~20–40%). These microstructures contribute to the rubber-like quasi-static and cyclic mechanical properties of both materials, with young’s moduli ranging from 1.8 to 13.2 MPa and extension to failure exceeding 250% over a range of strain rates (10–1−102 min−1). Finally, we discuss the potential for LRS and MRS ink components to be reclaimed and recycled, as well as be synthesized in resource-limited, extraterrestrial environments.