Abstract: Methods of making improved bioelectrodes are provided capable of functionalizing electrode materials in less than 24 hours. Pre-seeding the electrode with electricigenic microbes forms an electricigenic biofilm on the electrode to maximize surface coverage by electricigenic microbes and reduce the number of fastidious organisms. The method results in bioelectrodes that are functionalized in less than 24 hours and that can generate higher yields of current from a wide range of substrates. Methods for treating wastewater by removing fermentative inhibitors and generating current are provided. The bioelectrodes generated are tailored to efficiently oxidize substrates, such as the fermentative inhibitors, in the wastewater targeted for removal from the wastewater. Improved electrodes are generated rapidly with high coulombic efficiency. Bioelectrochemical systems (BESs) containing the improved electrodes are also provided.