Ni-NP/Ni anodes with varying Ni:NP ratio were prepared by electrodeposition of a thin Ni-NP (Nickel-Natural Phosphate) catalyst layer onto Ni plate for a direct methanol fuel cell (DMFC). The morphology and structure of the catalyst layers were analyzed by TEM and EDX. The catalyst coating layer shows an alloy character. The results show that these electrodes are very active for the methanol oxidation and that the optimum Ni: NP surface coverage was 50: 50 at % for DMFC operating at room temperature.