Eight different oxygen carriers (OC) containing CuO (60 wt %) and different mass ratios of CaO to Al2O3 as the support were synthesized by wet-mixing followed by calcination at 1000 °C. The method of synthesis used involved the formation of calcium aluminum hydrate phases and ensured homogeneous mixing of the Ca2+ and Al3+ ions in the support at the molecular level. The performance of the OCs for up to 100 cycles of reduction and oxidation was evaluated in both a thermogravimetric analyzer (TGA) and a fluidized bed reactor, covering a temperature range of 800 to 950 °C. In these cycling experiments, complete conversion of the OC, from CuO to Cu and vice versa, was always achieved for all OCs. The reactivity of the materials was so high that no deactivation could be observed in the TGA, owing to mass transfer limitations. It was found that OCs prepared with a mass ratio of CaO to Al2O3 in the support >0.55 agglomerated in the fluidized bed, resulting in an apparent deactivation over 25 cycles for all temperatures investigated. High ratios of mass of CaO to Al2O3 in the support resulted in CuO interacting with CaO, forming mixed oxides that have low melting temperatures, and this explains the tendency of these materials to agglomerate. This behavior was not observed when the mass ratio of CaO to Al2O3 in the support was ≤0.55 and such materials showed excellent cyclic stability operating under redox conditions at temperatures as high as 950 °C.