The purification treatment of carbon nanotubes-alumina was carried out using various oxidizers (ox), such as H2O2, concentrated HNO3, and air. The obtained composite was used as support for ruthenium catalysts. The structures and properties of the products before and after modification were characterized and measured using transmission electron microscopy (TEM), thermogravimetric analysis (TG), X-ray diffraction (XRD), and Fourier transform infrared (FTIR) spectroscopy. The results show that purification modification treatment can remove the impurities on the surface of the CNTs-alumina, shorten the CNTs, and increase the amounts of hydroxyl, carboxyl, and carbonyl groups. Inductively coupled plasma (ICP) analysis shows that the dissolution solution composition of the CNTs-alumina composite supports with HNO3 oxidation treatment contains 49.98 mg.g(-1) Al. The ammonia synthesis rate of the Ru/CNTs-alumina-H2O2 was found to be 39.8 mmol.g(-1).h(-1) at 10 MPa, 10000 h(-1), and 425 degrees C, which was higher than those for other CNTs-alumina-ox supported Ru catalysts.