Microbial fuel cells (MFCs) are potentially used for electricity generation, but their low power output hinders their practical application. This study presents novel, porosity binderless PPy-CS-CNT hydrogel materials, which were prepared using Fe(NO3)(3) as an initiator. It can be seen from the results of SEM and swelling ratio that the prepared material had a uniform structure with rich three-dimensional porosity and showed good water retention performance. Electrochemical tests showed that the charge transfer impedance (R-ct) of PPy-CS-CNT anode displayed a reduction in comparison with PPy anode (1.06 Omega vs. 2.20 Omega). And the power density of MFC with PPy-CS-CNT anode reached 364 mW m(-2), which was 1.36 times as much as that of MFC with PPy anode. High-throughput sequencing results showed that the PPy-CS-CNT hydrogel bioanode exhibits good biocompatibility and selective enrichment of electrogenic bacteria. The dominant genera on PPy-CS-CNT hydrogel anode are the electroactive bacteria, Rhodopsedomonas (47.69%) and Geobacter (8.47%). Therefore, the PPy-CS-CNT hydrogel anode showed a potential for improving the electricity production performance of MFCs. (C) 2019 Elsevier Ltd. All rights reserved.