Advances in carbon dioxide removal technology for spacecraft air revitalization promise to reduce the size and power consumption of carbon dioxide removal systems on future space missions. AlliedSignal has developed a Functionalized Carbon Molecular Sieve (FCMS) that can simultaneously remove carbon dioxide and water vapor. A thermally-coupled pressure-swing adsorption system has been designed using FCMS as the sorbent to provide regenerative carbon dioxide removal. The low regeneration temperature of FCMS results in lower power consumption than is required for conventional adsorbents, which typically desorb carbon dioxide at higher temperatures. The thermally-coupled pressure-swing system was tested, and results were compared to the Space Station Carbon Dioxide Removal Assembly (CDRA) as a reference design. The comparison indicated that a thermally-coupled pressure-swing system with FCMS offers significant savings in mass, volume and power consumption.