Fostering the creation of clean energy technologies that eliminate gas emissions and positively impact the environment is vital for confronting the dual challenges of escalating energy demands and environmental contaminants. Membrane-based technologies have emerged as effective strategies for harvesting clean energy and practically purifying water from contaminated wastewater. Here, we show that polyvinylidene difluoride (PVDF) with functionalized molybdenum disulfide (sMoS2) and nanocellulose (NC) is an attractive membrane for single-chamber air cathode microbial fuel cells (MFCs). Compared with conventional proton exchange membranes, our membrane boosts power generation up to 48.5 mW m−2 and efficiently catalyzes sonocatalytic dye degradation with 96 % efficiency when treating wastewater. This performance is due to a relatively high hydrophilicity, ion exchange capacity (0.84 meq. g−1), and proton conductivity (1.03 × 10−2 S cm−1), combined with reduced oxygen permeability (27 × 1012 cm s−1) compared with conventional membranes. The synergy effect of the PVDF matrix and sMoS2 + NC promotes proton transfer, enhancing electricity generation and pollutant degradation. The membrane shows promising stability and mechanical properties, offering a viable membrane for improved energy recovery from wastewater treatment.