Adsorptive separation of water from CO 2 is an appealing alternative to liquid absorbers for post-combustion capture systems. In all cases, the purified CO 2 stream from a PCC system will have a high moisture content and, due to equipment corrosion issues and the risk of hydrate formation, the CO 2 stream must be rigorously dried prior to being compressed. This work reports the first study on solid adsorbent selection for CO 2 drying using low grade heat and ambient air as a regeneration gas. Different types of adsorbents, chosen for their range of water adsorption characteristics, have been investigated for the desiccation of a pure CO 2 stream. When destined for sequestration the CO 2 product gas has little value and so the drying process should require no supporting process operations and should consume little additional energy. However, due to the costs and complexity of separating and purifying CO 2 from a flue gas stream, the drying process should return as much CO 2 as possible to the compression stage. An ideal desiccant for CO 2 drying should have a high moisture capacity and selectivity and should be regenerable using waste heat and ambient, humid air. The CO 2 drying performance of Na-, Ca-, and Ca/H- forms of ETS-10 were compared to that of commercial silica and 4A zeolite. Ca-ETS-10 was found to have the highest moisture capacity using a temperature swing of 30–70°C and a CO 2 feed stream of 50–100% relative humidity. Due to the intrinsic selectivity for water over CO 2 on solid adsorbents, all desiccants tested had a CO 2 recovery greater than 95%.