In this study, the integration of the electrocoagulation (EC) process with anaerobic digestion as a novel in-situbiomethanation approach was considered for the first time. As a result of this integration (iron electrodes, current density of 1.5 mA/cm2 and an exposure mode of 10-min-ON/ 30-min-OFF) the carbon dioxide content of biogas reached below 2%. Also, the methane production rate improved by 18.0 ± 0.4%, whereas the removal efficiencies of chemical oxygen demand, turbidity, phosphate, and sulfate increased by 12.0 ± 1.5%, 30.7 ± 1.7%, > 99%, and 75.7%, respectively. Anaerobic granular sludge characteristics were also improved. Moreover, the EC process stimulated growth and quantity of functional microorganisms, especially Acinetobacterin bacterialandMethanobacteriumin archaeal community. Methane concentration, however decreased due to possible excess hydrogen production. The application of the biogas as bio-hythane, and the optimization of the hybrid bioreactor to decrease hydrogen production, are possible avenues for further research.