Chemical looping auto-thermal reforming (CLATR) of methanol is an energy-efficient route for low-temperature methanol conversion to produce hydrogen. The construction and modulation of redox catalysts for selective hydrogen generation is the main challenge in this chemical looping processes. This paper describes the design of CuO/CeO₂/Al₂O₃ redox catalysts for chemical looping methanol conversion. It is found that the lattice oxygen atoms of copper oxides are involved in the complete oxidation of methanol to produce heat for auto-thermal reforming. The interfacial oxygen species over CuO/CeO₂/Al₂O₃ redox catalysts participate in the partial oxidation stage to facilitate the oxidation of methoxy to formate species, which is the key step in the methanol conversion process, boosting the hydrogen production in the CLATR process. The average H₂ production rate can reach 34.7 umol/(g_cat•s) and the average CO selectivity goes down to 0.35% per cycle at 220 ℃ with a H₂O/CH₃OH ratio (S/C) of 0.5 in the CLATR process. This study provides a promising strategy for selective hydrogen production.