The effect of regeneration conditions on the cyclic sorption-enhanced steam reforming of ethanol (SESRE) in a fixed-bed reactor was investigated. Columnar Ni–Ca catalysts were used in the cyclic SESRE experiments. The effects of different parameters, including temperature, purge direction, and purge gas on the regeneration process were discussed. The experimental results reveal that the regeneration temperature strongly affected not only the CO2 desorption rate but also the durability of the CaO sorbent. The stability of the CaO sorbent within the Ni–Ca catalyst was improved owing to the formation of Ca12Al14O33. Moreover, the type of purge gas (N2 or air) for regeneration had negligible effect on the CO2 capture performance of the Ni–Ca catalyst. For regeneration by air purging, coke decomposition over the Ni–Ca catalyst was accompanied by a slight decline in the activity of the Ni catalyst, which was attributed to the cyclic Ni redox.