This study demonstrated the enhancement of biogenic coal conversion to methane in a bioelectrochemical anaerobic reactor with polarized electrodes. The electrode with 1.0 V polarization increased the methane yield of coal to 52.5 mL/g lignite, which is the highest value reported to the best of our knowledge. The electrode with 2.0 V polarization shortened the adaptation time for methane production from coal, although the methane yield was slightly less than that of the 1.0 V electrode. After the methane production from coal in the bioelectrochemical reactor, the hydrolysis product, soluble organic residue, was still above 3600 mg chemical oxygen demand (COD)/L. The hydrolysis product has a substrate inhibition effect and inhibited further conversion of coal to methane. The dilution of the hydrolysis product mitigates the substrate inhibition to methane production, and a 5.7-fold dilution inhibited the methane conversion rate by 50%. An additional methane yield of 55.3 mL/g lignite was obtained when the hydrolysis product was diluted 10-fold in the anaerobic toxicity test. The biogenic conversion of coal to methane was significantly improved by the polarization of the electrode in the bioelectrochemical anaerobic reactor, and the dilution of the hydrolysis product further improved the methane yield.