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To understand how granular activated carbon (GAC) promotes methanogenesis, batch tests of CH₄ production potential in anaerobic serum bottles with addition of GAC or not were conducted. Tests showed that GAC promoted methanogenesis remarkably, but the non-conductive zeolite did not. The qPCR demonstrated that the biomass on GAC contributed little to the promotion. High-throughput sequencing data implied that promotion was related with direct interspecies electron transfer between Geobacteraceae and Methanosaetaceae. According to the c-type cytochromes (c-Cyts) response to the supplement of GAC, it was speculated that GAC may play the role of c-Cyts’ substitution. In the undefined cultures, the phenomenon that c-Cyts were repressed by GAC was first observed. This research provided new evidence to microbial mechanism of promoting methanogenesis via GAC.