The effects of bioelectrochemical systems (BESs) for the suppression of methane gas emissions from sediment were examined using a laboratory-scale reactor system. Methane gas emissions from acetate were suppressed by approximately 36% from control based on the installation of a BES in which carbon-graphite electrodes were buried in sediment and arbitrarily set at certain oxidative potentials (+300 mV vs Ag/AgCl) using a potentiostat. Meanwhile, methane gas emissions increased in the BES reactor where the electrode potential was set at -200 mV. Results obtained from pyrotag sequencing analysis of the microbial community on the surface of the buried electrodes targeting 16S rRNA genes demonstrated that the genusGeobacterhad drastically propagated in a sample from the reactor where the electrodes were buried. Quantitative analysis of 16S rRNA genes of archaea also revealed that the archaeal population had decreased to approximately 1/6 of its original level on the electrode of the BES set at +300 mV. This implied that the oxidation-reduction potential (ORP) in the sediment was raised to the inhibition level for methanogenesis in the vicinity of the buried electrode. Analysis of electron flux in the experiment revealed that electrons intrinsically used for methanogenesis were recovered via current generation in the sediment where a potential of +300 mV was set for the electrode, although most electrons donated from acetate were captured by oxygen respiration and other electron-accepting reactions. These results imply that BES technology is suitable for use as a tool for controlling re-dox-dependent reactions in natural environments, and that it also brought about changes in the microbial population structure and methanogenic activity in sediment.