Developing high-active and low-cost bifunctional materials for catalyzing hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) holds pivotal role in water splitting. Therefore, we present a new strategy to form NiS/Ni2P heterostructures. The as-obtained NiS/Ni2P/CC requires overpotentials of 111 mV for the HER and 265 mV for the OER to reach a current density of 20 mA cm-2, outperforming their counterparts such as NiS and Ni2P under the same conditions. Additionally, the NiS/Ni2P/CC electrode requires a 1.67 V cell voltage to deliver 10 mA cm-2 in two-electrode electrolysis system, which is comparable to the cell using the benchmark Pt/C||RuO2 electrode. Detailed characterizations reveal that strong electronic interactions between NiS and Ni2P, abundant active sites, and smaller charge transfer resistance contribute to the improved HER and OER activity.