In this study, a novel Al°-CNTs-Cu2O composite, capable of activating O2 to generate H2O2 and further to reactive oxygen species (ROSs) at a wide pH range, was synthetized, characterized and applied for the degradation of sulfamerazine. In the activation of O2 by Al°-CNTs-Cu2O composite, H2O2 was generated from the reaction of O2 with Al°-CNTs, which could be catalytically decomposed into O2− and OH by Cu2O, the formed Cu(II) could be rapidly reduced to Cu2O by Al°-CNTs in composite, which made Al°-CNTs-Cu2O composite reusable and decreased the leaching of copper ions into solution. The removal efficiency of SMR and TOC was 73.91 % and 56.80 %, respectively at initial pH = 5.8, T = 20 °C, O2 flow rate = 100 mL/min, Al°-CNTs-Cu2O dosage = 2 g/L, SMR = 50 mg/L, and reaction time = 60 min. The removal efficiency of SMR kept almost unchanged and the concentration of copper ions in solution was below 0.5 mg/L. The Al°-CNTs-Cu2O/O2 process could be used as a novel catalyst for the degradation of refractory organic contaminants in water and wastewater by Fenton-like process at a wide pH range through the in situ generation of H2O2.