Ion-beam modification of materials whose service properties are mainly controlled by the surface composition is of especial interest, in particular, for electrocatalysts, namely electrodes of fuel cells — perspective chemical current sources. A catalyst is needed for effective operation of fuel cell. In this paper active layers of the electrocatalysts were prepared by ion beam assisted deposition of catalytic (platinum) and activating (cerium) metals onto carbon (AVCarb® Carbon Fiber Paper P50 and Toray Carbon Fiber Paper TGP-H-060 T) catalyst supports. Formation of layers by ion beam assisted deposition by means of the deposition of metal and mixing of precipitating layer with the substrate by accelerated ions of the same metal, was carried out. Metal deposition and mixing between the precipitable layer and surface of the substrate by accelerated (U = 10 kV) ions of the same metal were conducted from a neutral vapor fraction and plasma of vacuum arc discharge of a pulsed electric arc ion source. Study of the morphology and composition of layers was carried out by the scanning electron microscopy, energy dispersive X-ray microanalysis, X-ray fluorescence analysis, and the Rutherford backscattering spectrometry methods. According to the investigations with the use of cyclic voltammetry, the electrocatalysts with the prepared layers exhibited catalytic activity in the reactions of electrochemical oxidation of methanol and ethanol, which form the basis for the principle of operation of low temperature direct methanol and direct ethanol fuel cells.