The objective of this research is to investigate the effect of different aerogel supports on the stability of copper oxide during limited cycles of CH 4 chemical looping combustion (CLC) in a thermogravimetric analyzer (TGA). Supports proved to be significantly effective not only for the fuel utilization efficiency of CLC but also for the stability of the oxygen carrier (OC). The evaluation tests were performed by employing CuO/aerogel (zirconia, alumina, and silica) OCs synthesized utilizing a novel patented method. The results showed that the OC prepared using zirconia aerogel support had the highest activity over a medium-temperature range (550−800 °C). The OCs were characterized using different methods, including surface area and pore analysis, TGA, X-ray diffraction (XRD), scanning electron microscope (SEM), and dynamic light scattering analysis. The results demonstrated that the proper support can stabilize Cu dispersion, intensify the redox degree of OCs at high temperatures, and strengthen the distribution of Cu on the surface of the support.