Greywater reuse has emerged as a promising solution for addressing water shortages. However, greywater needs treatment before reuse to meet the required water quality standards. Conventional wastewater treatment technologies are unsuitable for recreating highly decentralized domestic greywater. This study evaluated bioelectrochemical reactors (BERs) with granular activated carbon (GAC) as a sustainable alternative for developing decentralized and low-cost biological treatment systems. BERs using GAC as the anode material and conventional GAC biofilters (BFs) for synthetic greywater treatment were operated in batch mode for 110 days in two stages: (i) with polarized anodes at −150 mV vs. Ag/AgCl and (ii) as a microbial fuel cell with an external resistance of 1 kΩ. Anode polarization produced an electrosorption effect, increasing the ion removal of the BERs. Power production during the operation and cyclic voltammetry tests of the extracted granules revealed electrochemically active biofilm development on the BERs. Although low power density (0.193 ± 0.052 µW m−3) was observed in BERs, they showed a similar performance in sCOD removal (BER = 91.6–89.6 %; BF = 96.2–93.2 %) and turbidity removal (BER = 81–82 %; BF = 30–62 %) to BFs that used 50 % aeration. Additionally, scanning electron microscopy of sampled granules showed higher biomass formation in BER granules than in BF granules, suggesting a higher contribution of sessile (vs. planktonic) cells to the treatment. Thus, the results highlight the synergistic removal effect of the GAC-based BER. The scalable design presented in this study represents a proof-of-concept for developing BERs to use in decentralized greywater treatment systems.