Both narrow size and highly homogeneous distribution of Pt and PtRu nanoparticles (NPs) are achieved on multi-walled carbon nanotubes functionalized by perylene diimide derivatives (PD-CNTs) using ethylene glycol as reducing agents. FT-IR and UV-visible spectrum illustrate that the PA molecule has been successfully transformed into PD molecule and modified on the surface of CNTs. TEM images show that a multilayer of the PD moiety is formed on CNT surface followed by the uniform deposition of Pt and PtRu NPs through self-assembly. The resulting Pt and PtRu NPs on PD-CNTs exhibit competitively catalytic activity for methanol electro-oxidation and outstanding CO-tolerance properties compared to PtRu NPs on acid-oxidized CNTs (AO-CNTs) and carbon black. Furthermore, the PD-CNT based catalysts are also much more stable than PtRu/AO-CNTs through long-term cycle stability testing. The proposed synthesis route provides a facile, feasible and effective method for developing highly efficient electrocatalysts. 2013 (C) Elsevier B.V. All rights reserved.