A copper-based catalyst supported on carbon microspheres prepared by using the spray drying method has exhibited interesting Fenton-like catalytic properties for the degradation of Methyl Orange, Methyl Blue, and Rhodamine B in aqueous solution. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) data suggested that the catalyst consisted of copper particles covered by cuprous oxide. The influence of initial pH, reaction temperature, dosage of catalyst, and H2O2 concentration on the catalyst performance were investigated. Under optimum reaction conditions, the Behnajady-Modirshahla-Ghanbery kinetics model was observed to fit well with the experimental data. It was also observed that hydroxyl radical (HO center dot) formed from the reaction between hydrogen peroxide (H2O2) and cuprous (Cu+) species was responsible for the dye degradation under acidic conditions. This work provides new insights into the mechanism and kinetics of low-valence copper-carbon composite Fenton like catalyst for degrading organic dyes.