As the support of Pt and Pt-Ru catalysts for ethanol electrooxidation, the ethylenediamine (ED)-grafted multiwalled carbon nanotubes (MWNT) were prepared by a chemical synthesis method and characterized by Fourier transform infrared spectroscopy. The morphology and elemental composition of the Pt-Ru/ED/MWNT and Pt/ED/MWNT catalysts were characterized by transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy. TEM results demonstrate that the ED-grafted MWNT is beneficial to loading Pt-Ru and Pt electrocatalysts with well dispersion and small particle sizes. On the other hand, the electrocatalytic properties of the Pt-Ru/ED/MWNT and Pt/ED/MWNT catalysts were characterized by cyclic voltammetry and chronoamperometry. Under the same loading mass of catalyst, the electrocatalytic activities of both Pt-Ru/MWNT/graphite and Pt/MWNT/graphite electrodes are enhanced obviously by the introduction of ED. The electrocatalytic activity of the Pt/ED/MWNT/graphite electrode is even higher than that of the Pt-Ru/MWNT/graphite electrode. These results indicate that the ED/MWNT is a promising catalyst support for ethanol electrooxidation.