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Processes to remove and recover carbon dioxide (CO2) and water vapor from air are essential for successful long-duration space missions. This paper presents results of a developmental program focused on the use of a liquid-sorbent/membrane-contactor (LSMC) system for removal of CO2 and water vapor from air. In this system, air from the spacecraft cabin atmosphere is circulated through one side of a hollow-fiber membrane contactor. On the other side of the membrane contactor is flowed a liquid sorbent, which absorbs the CO2 and water vapor from the feed air. The liquid sorbent is then heated to desorb the CO2 and water vapor. The CO2 is subsequently removed from the system as a concentrated gas stream, whereas the water vapor is condensed, producing a water stream. A breadboard system based on this technology was designed and constructed. Tests showed that the LSMC breadboard system can produce a CO2 stream and a liquid-water stream. Details are presented on the operation of the system, as well as the effects on performance of variations in feed conditions.