In this work, platinum‐free based cathodes are investigated for their application in microbial fuel cells (MFCs). Carbon cloth and stainless steel grid were employed as different supporting materials for the electrodeposition of three types of inert carriers, for example, clay, silica, and aluminum‐nickel alloy, all of them combined with nickel. This work evaluates the potential of this technique in order to elaborate active MFC cathodes. The voltammograms obtained confirm both the reduction of protons, with the adsorption of hydrogen from −0.5 to −1.8 V, and the oxidation of water, producing sufficient current intensity to reduce oxygen. Among the options investigated, cathodes based on aluminum‐nickel alloy/nickel achieved the highest catalytic activity, being carbon cloth the most suitable supporting material. Thus, aluminum‐nickel alloy/nickel electrocodeposited onto carbon cloth exhibited the highest levels of power output (150 mW.m−3) when tested in MFCs fed with wastewater. This type of low cost cathodes also offers promising results for wastewater treatment reaching up to 90% of chemical oxygen demand removal. © 2018 American Institute of Chemical Engineers Environ Prog, 38:e13083, 2019