The application of chemical looping to reverse water gas shift and methane dry reforming provides an efficient way for converting CO2 to CO, enabling the transformation of captured CO2 into value-added products. For example, this can be achieved by using the produced CO along with renewable H2 to synthesise liquid fuels via the Fischer–Tropsch process. In this study, we applied the concept of a 'chemical memory reactor' proposed by Metcalfe et al., employing a perovskite-based oxygen carrier (La0.6Sr0.4FeO3-δ, LSF) in a counter-current packed-bed reactor for CO2 splitting. This approach overcomes the chemical equilibrium limitation of chemical-looping CO2 splitting and produces unmixed CO. Our work experimentally investigated the performance of LSF pellets as oxygen carriers in a large lab-scale packed-bed reactor with gas switching technology at SINTEF for chemical-looping CO2 splitting between 670 and 820 °C. We evaluated the effects of changes in feed time, bed temperatures, flow rates, and inlet gas concentrations on CO2 to CO conversion. Under representative conditions, the averaged CO2 to CO conversion was 44% for chemical-looping CO2 splitting with cocurrent flow and it increased to over 90% for chemical-looping CO2 splitting via counter-current flow over 50 cycles. Careful adjustment and control of feed time and flow rates could ensure high CO and CO2 conversions for both cycles. Our developed numerical model accurately predicted experimental results, indicating that nearly complete conversions can be achieved without thermodynamic limitations for chemical-looping CO2 splitting in such a reverse-flow memory reactor, utilising a non-stoichiometric LSF perovskite oxygen carrier material.