The Lunar Sulfur Capture System (LSCS) is an innovative method to recover sulfur compounds from lunar soil using sorbents derived primarily from in-situ resources. Most of the sulfur released from lunar soil during higher-temperature thermal treatment is trapped by the LSCS at lower temperatures on iron oxides present in lunar soil. As needed, small amounts of polishing sorbents are used to reduce equilibrium sulfur concentrations to the low ppm level. After sorbents become saturated, sulfur compounds are desorbed and converted to useful sulfur products. Sulfur is present in concentrations of about 0.1 percent in lunar soils and can be recovered by the LSCS as a useful product from in-situ resource utilization (ISRU). The LSCS can capture and recover sulfur from lunar soil as a primary product during thermal desorption of volatile compounds or during thermal reduction ISRU processes used for oxygen production. Removal of sulfur compounds is required during ISRU to prevent electrolyzer damage, catalyst poisoning, and equipment corrosion. The LSCS is applicable to thermal ISRU reduction processes in which sulfur is released in forms such as hydrogen sulfide (H2S), carbonyl sulfide (COS), or carbon disulfide (CS2).