Novel self-supported Mgy(CuxNi0.6-xMn0.4)1-yFe2O4 with (y = 0, 0.05, 0.1, 0.15, and x = 0, 0.15, 0.3, 0.45, 0.6) oxygen carriers (OCs) are synthesized through the co-precipitation method. The synthesized OCs’ properties are characterized by X-ray powder diffraction (XRD), Raman spectra, transform infrared spectroscopy (FT-IR), Brunauer-Emmett-Teller (BET), transmission electron microscopy (TEM), field emission scanning electron microscopy (FESEM), energy-dispersive X-ray spectroscopy (EDX), and Thermogravimetric Analysis (TGA). The synthesized OCs are assessed in Chemical Looping Steam Methane Reforming (CL-SMR) process subject to different mesh sizes, reaction temperatures, Steam/Carbon (S/C) molar ratios, Mg concentrations, and Cu and Ni concentrations. The characterization of the OCs and process results indicate the contributive effect of Mg incorporation on the CuxNi0.6-xMn0.4Fe2O4 support structure. The redox results reveal that Mg0.1(Cu0.3Ni0.3Mn0.4)0.9Fe2O4 OC is of the highest activity, even at low reduction temperatures. This OC exhibits the highest activity and stability with lowest coke deposition during 24 redox cycles at 650 °C and S/C = 2.5. The highest CH4 conversion of about 99.4% and H2 yield of about 84.4% are obtained.