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A biofilm anode acclimated with growth media containing acetate, then acetate + methane, and finally methane alone produced electrical current in a microbial electrochemical cell (MxC) fed with methane as the sole electron donor. Geobacter was the dominant genus for the bacterial domain (93%) in the biofilm anode, while methanogens ( Methanocorpusculum labreanum and Methanosaeta concilii ) accounted for 82% of the total archaeal clones in the biofilm. Fluorescence in situ hybridization (FISH) imaging clearly showed a biofilm of mixed bacteria and archaea, suggesting a syntrophic interaction between them for performing anaerobic oxidation of methane (AOM) in the biofilm anode. Measured cumulative coulombs were linearly correlated to the methane-gas concentration in the range of 10–99.97% (R 2 ≥ 0.99) when the measurement was sustained for at least 50 min Thus, cumulative coulombs over 50 min could be used to quantify the methane concentration in gas samples. [ABSTRACT FROM AUTHOR]