This study explored the synergistic effects of exogenous acyl homoserine lactones (AHLs) and microbial electrolysis (ME) on enhancing anaerobic digestion (AD) of low-quality biomass. The combined AHLs + ME strategy achieved a 79.50 % increase in cumulative methane production compared to the control, outperforming individual treatments. This enhancement was attributed to accelerated substrate degradation, selective enrichment of hydrogenotrophic methanogens (Methanobrevibacter, Methanobacterium, Methanofollis), and strengthened quorum sensing, electron transfer, and methane synthesis pathways. Metagenomic analysis revealed abundance upregulation of key genes involved in AHL synthesis (bjaI, rpaI, braI, rhiI) and sensing (solR, cepR, tofR), direct interspecies electron transfer (pilA, mtrC), and hydrogenotrophic methanogenesis (ftr, mvhD, vhuD, vhcD). This study offers a novel and sustainable strategy to optimize methane production from recalcitrant biomass, advancing AD-based waste-to-energy systems.