In this study, the degradation of alizarin green (AG) by Ti/PbO2 electrode and Ti/IrO2 + Ta2O5 electrode was investigated; specifically, the degradation efficiency was compared. The optimal conditions for degradation, as determined from the results, were as follows: an initial concentration of the pollutant (AG) of 100 mg/L, an electrolyte (Na2SO4) concentration of 0.1 mol/L, a current density of 30 mA/cm2, and a pH of 5.86. Under these optimal conditions, the AG removal rate and chemical oxygen demand (COD) removal rate were greater than 81.4% and 51.6%, respectively, by Ti/PbO2 electrode and Ti/IrO2 + Ta2O5 electrode after 70 min of degradation. In comparison with the mud-cracked surface of the Ti/IrO2 + Ta2O5 electrode, the Ti/PbO2 electrode showed higher stability for its pyramid crystal structure. Furthermore, during degradation, accelerated spalling phenomena were observed by SEM on the Ti/IrO2 + Ta2O5 electrode surface owing to the mud-cracked surface structure. As a result, a TiO2 passive film was formed, which lead to an increase in cell pressure and a decrease in the electrocatalysis ability of the Ti/IrO2 + Ta2O5 electrode.