Abstract: Platinum-based nanocomposites have been considered as one of the most promising catalysts for methanol oxidation reactions (MORs), which yet still suffer from low electrochemical activity and electron-transfer properties. Apart from van-der-Waals heterostructures, herein, we report a novel nanocomposite with the structure of Pt–Ru bimetallic nanoparticles covalently-bonded onto multi-walled carbon nanotubes (MWCNTs) (Pt–Ru@MWCNT), which have been successfully fabricated via a facile and green synthesis method. It is demonstrated that the Pt–Ru@MWCNT nanocomposite possesses much enhanced electrocatalytic activity with the electrochemical active surface area (ECSA) of 110.4 m²·g⁻¹ for Pt towards MOR, which is 2.67 and 4.0 times higher than those of 20wt% commercial Pt@C and Pt-based nanocomposite prepared by other method, due to the improved electron-transfer properties originated from M–O–C covalent bonds. This work provides us a new strategy for the structural design of highly-efficient electrocatalysts in boosting MOR performance.