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Biological methanation as a method of sector coupling between electric and gas grids is expected to be an integral part of the green energy change. Wastewater treatment plants (WWTPs) involving anaerobic digestion (AD) allow existing infrastructure to operate as energy conversion plants, to close carbon cycles and to generate long-term storable energy in the form of biomethane. Therefore, municipal raw sludge and additional organic residuals (co-substrates) are converted into biogas. Hydrogen is added to convert the carbon dioxide in the biogas into methane via biological methanation (BM). In this study, the energy amount that is convertible via BM in municipal digesters in Austria was calculated. The amount of energy, which can be transformed from electric surplus energy into biomethane, was assessed. Operational data from lab-scale digesters were combined with data from 28 Austrian full-scale wastewater treatment plants with AD. They represent 9.2 Mio population equivalents (PE), or 68% of Austria's municipal AD capacity for WWTPs > 50,000 PE (in sum, 13.6 Mio PE). Energy flows for BM including water electrolysis and anaerobic digestion were created on a countrywide basis. It was found that 2.9–4.4% (220–327 GWh·y−1) of Austria's yearly renewable electricity production (7470 GWh·y−1) can be transformed into biomethane via BM in municipal digesters. [ABSTRACT FROM AUTHOR]