The polymer-assisted melting infiltration method was used to finely disperse Ni, Fe and bimetallic Ni-Fe precursors in ordered mesoporous SBA-15 support. This approach allowed to obtain small Ni nanoparticles, in the order of 2 nm in size, with finely dispersed iron oxide surrounding metallic Ni, without evidence of Ni-Fe alloy formation. The catalysts were used in the HDO reaction of m-cresol at 300 °C and atmospheric pressure. The conversion of m-cresol was found to be dependent on Ni content, with the total reaction rate decreasing when Ni is partially replaced by iron. Toluene was the main product obtained for both, mono Ni and bimetallic Ni-Fe catalysts, thus suggesting that nickel nanoparticles when in the form of small sized particles, are the active sites for deoxygenation, independent on the presence of oxophilic iron site in their proximity. Such findings will serve for the further design of effective catalysts for the upgrading of lignin-derived bio-oil.