The objective of the research presented here was to determine the effectiveness of applying electrolysis in polluted sediment to enhance ammonia nitrogen (NH 3 −N) and phosphate phosphorous (PO 4 3−-P) removal from sediment and overlying water. A magnesium‑aluminum (Mg Al) alloy was used as the anode, and a titanium (Ti) mesh served as the cathode with a low-current of 40 mA (5 V) in polluted river sediment and overlying water. The total nitrogen (TN), NH 3 -N and nitrate nitrogen (NO 3 −-N) were mainly removed through the electro-oxidation and electro-reduction process and the highly pH and DO value caused by electrolytic reaction which could also enhance the removal of NH 3 -N through nitrifying bacteria. There was significant difference (p = 0.021) during the removal between electrolyzed sediment and sediment without electrolysis control. Approximately 253.47 ± 1.82 mg TN were removed using an electrolysis treatment on sediment since the initial TN concentration was about 1312 ± 104.37 mg/kg in the polluted sediment and about 14.91 mg TN per day was removed which was 4.62 times greater than that removed by non-electrolysis controls. As for P in the sediment, the results showed that the Mg- Al alloy anode mostly released Mg2+ ions to promote the removal of PO 4 3−-P in the sediment and overlying water; meanwhile, the electrodeposition of PO 4 3−-P on the Ti mesh cathode was used to enhance PO 4 3−-P removal and totally about 106.65 ± 0.23 mg TP was removed since the TP concentration was 607.68 ± 32.27 mg/kg. Notably, electrolysis promoted the transformation of sodium hydroxide-P (NaOH-P) fractions to ammonia chloride-P (NH 4 Cl-P), which improved the bioavailability of P. Through energy dispersive spectrometry (EDS) and Fourier transform infrared (FTIR) analysis, the precipitates of the Ti mesh cathode and the precipitates produced between the sediment and overlying water both contain Mg, Ca, Al and P. Electrolysis had little effect on the removal of organic carbon in the sediment (p = 0.64). Taken as a whole, this study suggested that electrolysis-driven N and P removal could be a sustainable technology for the management of polluted river sediments. • Mg Al alloy anode transformed phosphorus in sediment and overlying water. • Ti mesh cathode used to remove phosphorus in sediment and overlying water. • Cathodes increased the proportion of autotrophic denitrifiers in sediment. • Electrolytic reaction under 40 mA current with 5 V more conducive to N & P removal. • 14.91 mg TN per day removed from heavily polluted river sediment and overlying water. [ABSTRACT FROM AUTHOR]