A sorption-enhanced water-gas shift (SEWGS) system providing CO2-free synthesis gas (CO + H2) for jet fuel production from pure CO was studied. The water-gas shift (WGS) reaction was catalyzed by a commercial Cu/ZnO/Al2O3 catalyst and carried out with in-situ CO2 removal on a 20 wt% potassium-promoted hydrotalcite-derived sorbent. Catalyst activity was investigated in a fixed bed tubular reactor. Different sorbent materials and treatments were characterized by CO2 chemisorption among other analysis methods to choose a suitable sorbent. Cyclic breakthrough tests in an isothermal packed bed microchannel reactor (PBMR) were performed at significantly lower modified residence times than those reported in literature. A parameter study gave an insight into the effect of pressure, adsorption feed composition, desorption conditions, as well as reactor configuration on breakthrough delay and adsorbed amount of CO2. Special attention was paid to the steam content. The significance of water during adsorption as well as desorption confirmed the existence of different adsorption sites. Various reactor packing concepts showed that the interaction of relatively fast reaction and relatively slow adsorption kinetics plays a key role in the SEWGS process design at low residence time conditions.