Chemical-looping technology has been suggested as one of the most promising technologies for reducing the cost of CO2 capture using fossil fuels. This technology involves the use of an oxygen-carrier, which transfers oxygen from air to the fuel avoiding the direct contact between them. Oxygen carriers based on nickel have been the most extensively analyzed in the literature because of their good performance working at high temperatures (900–1100 °C). It is well-known that Ni catalyzes steam methane reforming (SMR) and water–gas shift (WGS) reactions, which are produced both in chemical-looping combustion (CLC) and chemical-looping reforming (CLR) processes. In this work, the catalytic activity of two Ni-based oxygen-carriers prepared by impregnation, NiO18-αAl2O3 and NiO21-γAl2O3, with respect to SMR and WGS reactions, have been determined in a fixed-bed reactor at different operating conditions. The catalytic activity was similar for both oxygen-carriers but lower than that exhibited by conventional Ni c...