A novel Cu-Zn-TiO 2 nanotube array (TNTA) polymetallic nanoelectrode, intended to improve the electrochemical nitrate removal efficiency, was fabricated. The nanoelectrode was fabricated by plating Cu onto a Ti nanoelectrode and then plating Zn onto the Cu/Ti bilayer electrode produced. The Ti nanostructures on the Cu-Zn-TNTA nanoelectrode surface gave the nanoelectrode a large specific surface area, and the Zn and Cu gave the nanoelectrode a high electrocatalytic activity for reducing nitrate. Scanning electron microscopy images showed that the Cu-Zn-TNTA polymetallic nanoelectrode had a honeycomb structure with spongy deposits. X-ray diffractometry results showed that the Cu-Zn-TNTA nanoelectrode predominantly contained Cu, O, Ti, and Zn. The nitrate removal efficiency of the Cu-Zn-TNTA nanoelectrode was 345.7% of the removal efficiency for a Ti nanoelectrode. The presence of NaCl allowed both the cathodic reduction of nitrate and the anodic oxidation of the ammonia and nitrite byproducts to be achieved with high removal efficiencies, especially using an IrO 2 anode. In the present of NaCl, nitrate removal rate was 93.4% in current density of 30 mA/cm 2 after 90 min. Nitrate was completely removed using the IrO 2 anode, and little ammonia was detected in the treated solution. The reduction efficiency increased slightly as the initial nitrate concentration increased through the range 20-100 mg/L, and the pH had little effect on the nitrate reduction efficiency. Water resource shortages have become increasingly serious in recent years, and are aggravated by groundwater pollution. Nitrate is an important groundwater pollutant, and removing nitrate from groundwater is attracting increasing amounts of attention.1 Major anthropogenic sources of nitrate in groundwater are industrial wastewater, domestic sewage, animal waste, nitrogen fertilizers, and other waste liquids.2-4 The World Health Organization has set a guideline maximum nitrate concentration in drinking water of 45 mg/L, and the European Union regulatory limit is 50 mg/L for regular potable water and 15 mg/L for water ingested by infants. [5][6][7] High nitrate concentrations in drinking water can seriously harm human health, impairing oxygen transport to the tissues. The ingestion of nitrate can cause several health problems, including congenital deformities, gastric cancer, high blood pressure, mental decline, thyroid disorders (e.g., goiter), and visual and auditory problems, which develop relatively slowly. [8][9][10][11][12][13] Attention has therefore been given to developing methods for removing nitrate from groundwater. Various methods have been proposed for the removal of nitrate such as biological, physicochemical, chemical and electrochemical. 4 Biological method has various disadvantages e.g. it need a long time to react, difficult to control, react incomplete will release of NO 2, N 2 O and NO x , produced a large number of biological sludge, requires a constant supply of the organic substrate. This limits the biological removal of nitrate app...