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[Display omitted] • A novel hybrid system based on AGS to enhance methanogenesis. • Improve functional genes of methanogenic (mcrA) and electric transfer (omcZ). • Regulated the dense structure of EPS in AGS. • (Fe(III)/Fe(II)) as an intermediate station of electron transfer. • Promoted resistance to membrane contamination. 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. [ABSTRACT FROM AUTHOR]