The core–shell structure has been widely acknowledged as an effective design strategy for oxygen carriers in the chemical looping oxidative dehydrogenation (CL-ODH) of ethane. In this work, a molybdenum-promoted CuMn2O4oxygen carrier with a core–shell structure was prepared and characterized. The interaction between MoO3and CuMn2O4during the preparation process results in the formation of a nonmolten shell MnMoO4that encapsulates CuMn2O4, thereby significantly enhancing its capacity for the selective oxidation dehydrogenation of ethane. Experimental results indicated that the presence of the MnMoO4shell increased the ethylene selectivity from below 10% to 80.7%. Additionally, the CuMn2O4@MnMoO4oxygen carrier still exhibits a high oxygen capacity of 11.3 wt % with an effective oxygen capacity of 3.1 wt %. Thirty redox cycle experiments demonstrated an exceptional performance in terms of multicycle reactions, with a high ethane throughput of 90 mL/gcat/cycle and 85% ethylene selectivity. The combination of a high oxygen capacity and nonmolten shell characteristics provides valuable insights for designing oxygen carriers for CL-ODH.