Biotic-abiotic　hybrid　systems　are　promising　technologies　to　enhance　methane　production　in　anaerobic　wastewater　treatment.　However,　the　dense　structure　of　the　extracellular　polymeric　substances　(EPS)　present　in　anaerobic　granular　sludge　(AGS)　poses　challenges　with　respect　to　the　implementation　of　hybrid　systems　and　efficient　interspecies　electron　transfer.　In　this　study,　the　use　of　AGS　with　a　Ni/Fe　layered　double　hydroxide@activated　carbon　(Ni/Fe　LDH@C-AGS)　was　investigated　in　an　anaerobic　membrane　bioreactor　(AnMBR).　The　hybrid　system　showed　a　significant　increase　of　82%　in　methane　production.　Further　research　revealed　that　Ni/Fe　LDH@C　regulated　the　dense　structure　of　EPS,　stimulated　the　production　of　cytochromes,　and　facilitated　the　decomposition　of　nonconductive　substances.　Surprisingly,　the　hybrid　system　also　promoted　resistance　to　membrane　fouling　and　extended　membrane　life　by　81%.　This　study　provides　insights　into　the　operation　of　a　biotic-abiotic　hybrid　system　by　regulating　the　dense　structure　of　EPS　ultimately　resulting　in　an　enhanced　methane　production.