The critical issue for lunar construction lies in designing lunar habitats within the limits of harsh lunar environments and an extreme lack of construction resources. Inflatables, known for their versatility in space habitats, are a promising concept due to their adaptability to transportation, stowage, and reliability challenges. Rigidization technologies significantly enhance the safety, durability, and repairability of these structures. Our prior work introduced a rigidizable inflatable lunar habitat utilizing composite materials as restraint layers and shape memory polymers (SMP) for rigidization. Temperature influences resin stiffness, affecting the folding performance of the membrane. Folding, even in the flexible state, poses a risk of resin damage, compromising the structure’s load-bearing capacity. This paper presents an optimal material, silicon-coated aramid fabric (SC-AF), exhibiting superior mechanical properties over the previously proposed flexible aramid fiber reinforced polymer (AFRP) (comprising Kevlar fiber fabric and flexible epoxy resin). Through uniaxial tensile, puncture, and tearing tests, the new material demonstrates enhanced stability, folding capability, and good tearing resistance. After folding, the SC-AF specimens show a 17% stiffness reduction with negligible impact on material strength. This reduction may be attributed to fiber deformation and misalignment, as well as local buckling and micro-cracks in the silicon coating. These factors lead to decreased fiber alignment during tension, ultimately resulting in a softening effect. Future studies will quantitatively investigate stiffness reduction and assess long-term material properties under simulated lunar environments. The pursuit of advanced materials and rigidization methods will persist to facilitate efficient construction in extreme environments.