Our research staff has been able to perform long-term operation of a 200 kW gas-circulating combustion system successfully for over 100 h with NiO/Al 2 O 3 oxygen carrier particles that were produced in large quantities using a pilot-plant spray dryer. After such a result, we are planning to scale-up the process to a 1−10 MW system. Iron oxide, which is relatively cheaper than expensive NiO, has been considered for this step, and nine different types of NiO/Fe 2 O 3 /Al 2 O 3 mixed metal oxides were produced by adding iron oxide to NiO with a 22.5−47.5 wt % ratio, adding 30 wt % Al 2 O 3 as support, and finally, forming material using the spray-drying method. Results from both physical property tests [tapping density, particle size analysis, attrition index (AI), porosity analysis, and Brunauer−Emmett−Teller (BET) surface area] and chemical property tests [scanning electron microscopy (SEM), electron probe X-ray microanalysis (EPMA), and X-ray diffraction (XRD)] suggest that a mixed metal oxide of 22.5 wt % NiO, 47.5 wt % Fe 2 O 3 , and 30 wt % Al 2 O 3 calcined at 1100 °C is suitable for the fluidized-bed process with excellent oxygen-transfer capability. Oxygen-transfer capability was higher than the theoretical value of N1F2 particles, and it can be explained as spinel Ni(Al,Fe) 2 O 4 solid solution through XRD analysis. It is believed that mixed metal oxides produced are good candidates for media-circulating combustion of the fluidized-bed process for the large capacity of a 1−10 MW system for the future. Because oxygen-transfer capability of the mixed metal oxides was maintained without degradation after multiple cycles and despite the oxidation rate being relatively slow, the reduction rate was very fast.