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[Display omitted] • Three cathode materials were compared for CH 4 and acetate bioelectrosynthesis. • Carbon felt cathode showed the highest CH 4 production per cathode volume. • Conductive polymer cathode promoted acetate and ethanol production. • Cathode material selection affects biofilm activity and bioelectrosynthesis pathways. This study compares carbon felt (CF), granular activated carbon (GAC), and a conductive acrylonitrile butadiene styrene (cABS) polymer cathodes for CH 4 and acetate production in a microbial electrosynthesis (MES) cell. At an applied voltage of 2.8 V and continuous CO 2 flow, the CF biocathode MES cell showed the highest CH 4 production rate of 1420 ± 225 mL V c -1 d-1 (V c = cathode volume), also producing acetate at a rate of 710 ± 110 mg V c -1 d-1. The volumetric rates of acetate and CH 4 production decreased when using the GAC cathode (720 ± 94 mL V c -1 d-1 and 236 ± 65 mg V c -1 d-1, respectively). When the cABS cathode was used, the CH 4 production declined to 250 ± 35 mL V c -1 d-1, while the acetate production increased to 1105 ± 130 mg V c -1 d-1. The biocatalytic activity of cABS increased after in-situ electrodeposition of Ni and Fe, resulting in a current increase from 205 mA to 380 mA accompanied by increasing acetate and ethanol production (1405 mg V c -1 d-1 and 240 mg V c -1 d-1, respectively), while the CH 4 production decreased. The cABS cathode showed the highest specific (per surface area) activity for acetate and CH 4 production. [ABSTRACT FROM AUTHOR]