Pt-Ru catalysts based on functional polymer-grafted MWNT (Pt-Ru@FP-MWNT) were prepared by radiolytic deposition of Pt-Ru nanoparticles on functional polymer-grafted multiwalled carbon nanotube (FP-MWNT). Three different types of functional polymers, poly(acrylic acid) (PAAc), poly(methacrylic acid) (PMAc), and poly(vinylphenyl boronic acid) (PVPBAc), were grafted on the MWNT surface by radiation-induced graft polymerization (RIGP). Then, Pt-Ru nanoparticles were deposited onto the FP-MWNT supports by the reduction of metal ions using γ-irradiation to obtain Pt-Ru@FP-MWNT catalysts. The Pt-Ru@FP-MWNT catalysts were then characterized by XRD, XPS, TEM ,and elemental analysis. The catalytic efficiency of Pt-Ru@FP-MWNT catalyst was examined for CO stripping and MeOH oxidation for use in a direct methanol fuel cell (DMFC). The Pt-Ru@PVPBAc-MWNT catalyst shows enhanced activity for electro-oxidation of CO and MeOH oxidation over that of the commercial E-TEK catalyst.