A series of MgAlFeCu mixed oxides with different chemical compositions derived from hydrotalcite-like compounds were prepared by the NaAlO2-coprecipitation method and characterized by XRF, XRD, and N-2 adsorption analysis. These sulfur-transfer catalysts were evaluated as SOx removal catalysts under the conditions similar to those of FCC units. The results showed that the total SO2 adsorption amounts increased with increasing magnesium content. And the redox properties of Fe2O3 enhanced significantly the adsorption-reduction capacities of the catalysts, while CuO can be used as an effective oxidation promoter. Furthermore, the catalyst LDOs-6 (Mg/Al = 6, Fe2O3% = 8% and CuO% = 1%) presented the excellent SO2 removal capacity, its total amounts of adsorbed SO2 reached 1.74 g /g in 7 min, which also remained constant after eight cycles. These results indicated that the performances of the catalysts were closely related to the chemical composition.