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NASA’s Artemis Program seeks to establish a long-term presence on the Moon to enable scientific exploration and expand the cis-lunar economy by utilizing lunar resources through public-private and international partnerships. Over the next decades, a lunar spaceport will need to be established to provide the services and facilities that are necessary to achieve this goal. Robotic construction technologies using in-situ materials must be developed to build up enabling infrastructure such as launch/landing pads, blast protection, power/communications infrastructure, improved roads, improved operational surfaces, and radiation protection shelters. Kennedy Space Center’s Granular Mechanics and Regolith Operations laboratory at Swamp Works has partnered with SpaceFactory and LERA Consulting Structural Engineers to develop the architectural and structural design of an unpressurized lunar shelter. The shelter, called Lunar Infrastructure Asset (LINA), is designed to support 2.3 m of regolith overburden to protect astronauts and surface assets from radiation, meteoroid impact, thermal gradients/cycling, and to withstand moonquakes. LINA’s structural design criteria and the resulting structure design are detailed in separate papers. A Fused Filament Fabrication (FFF) construction process using regolith polymer composites has been developed and is detailed in a separate publication. This paper presents material formulations and selection rationale for each of the composite components that were examined. Formulations include 70:30, 80:20, and 85:15 wt.% mixture ratios of lunar mare simulant Black Point-1 (BP-1): Polylactic Acid (PLA), 80:20 Lunar Highlands Simulant-1 (LHS-1): PLA and an 80:20 BP-1: PLA formulation with a flow enhancer additive. Test samples were printed in simulated lunar dirty thermal vacuum conditions (-190 °C, 10-3 torr). A series of tests were performed on each formulation to characterize the achieved mixture ratio, mechanical strength properties, off-gassing products during vacuum printing, and porosity and density of printed products. The LHS-1: PLA formulation yielded an advantageous combination of properties and was used in a final test that additively constructed a sub-scaled LINA on regolith simulant in dirty vacuum conditions. The materials and construction process presented in this paper are considered to be at Technology Readiness Level (TRL) 5 with additional testing necessary to characterize long term lunar environmental exposure effects.