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PtRu nanoparticles with a diameter of 10–15 nm were electrodeposited within multiwalled carbon nanotube-Nafion (MWCNT-Nafion) nanocomposite. The formation of PtRu nanoparticles in MWCNT-Nafion nanocomposite was characterized by scanning electron microscopy, transmission electron microscopy, and energy dispersive X-ray spectroscopy. The electrocatalytic activity towards the methanol electrooxidation at PtRu-MWCNT-Nafion and Pt-MWCNT-Nafion nanocomposite-modified glassy carbon electrodes was investigated by cyclic voltammetry. The results indicated that the PtRu-MWCNT-Nafion nanocomposite was electrocatalytically more active than Pt-MWCNT-Nafion nanocomposite. The effect of atomic ratio of Pt : Ru on the electrocatalytic ability towards the methanol electrooxidation was investigated in order to achieve a high catalyst use. The PtRu bimetallic catalyst with 1 : 1 atomic ratio showed better electrocatalytic activity towards the methanol electrooxidation. The stability for the methanol electrooxidation at PtRu-MWCNT-Nafion nanocomposite modified was also investigated.