Capturing carbon dioxide is vital for the future of climate-friendly combustion, gasification, and steam-reforming processes. Dry processes utilizing simple sorbents have great potential in this regard. Long-term calcination/carbonation cycling was carried out in an atmospheric-pressure thermogravimetric reactor. Although dolomite gave better capture than limestone for a limited number of cycles, the advantage declined over many cycles. Under some circumstances, decreasing the carbonation temperature increased the rate of reaction because of the interaction between equilibrium and kinetic factors. Limestone and dolomite, after being pretreated thermally at high temperatures (1000 or 1100 degrees C), showed a substantial increase in calcium utilization over many calcination/carbonation cycles. Lengthening the pretreatment interval resulted in greater improvement. However, attrition was significantly greater for the pretreated sorbents. Greatly extending the duration of carbonation during one cycle was found to be capable of restoring the CO2 capture ability of sorbents to their original behavior, offering a possible means of countering the long-term degradation of calcium sorbents for dry capture of carbon dioxide.