Pt/Ru deposited on multi-walled carbon nano-tubes (MWCNTs) was prepared with water/iso-propanol solutions containing Pt(IV) and Ru(III) ions by γ-irradiation. The water/iso-propanol ratio (v/v), additive amount of surfactant, the concentration ratio of Pt(IV)/Ru(III) ions and the total absorbed doses (kGy) were evaluated as synthesis parameters. The sample morphology was characterized by SEM and the Pt/Ru atomic ratio was obtained by EDX. It has been found that multi-walled carbon nano-tubes can be well distributed in the water/iso-propanol solution with additive of surfactant. Pt(IV) and Ru(III) ions can be reduced by both of hydrated electron and radical of iso-propanol produced from hydrogen abstraction reaction. The Pt/Ru atom ratio can be controlled by changing the ratio of Pt(IV)/Ru(III). Small nano-particles of Pt/Ru deposited on MWCNTs can be obtained for possible application of electro-catalysts in the proton exchange membrane fuel cells (PEMFC) under optimum conditions with absorbed doses, amount of surfactant, water/iso-propanol ratio and so on. The reduction of Pt(IV)/Ru(III) ions in the aqueous solution with additive of surfactant was also studied by use of pulse radiolysis and the mechanism involved in the reduction process has been proposed.