In this contribution, we demonstrate that electrodeposited nickel diselenide nanoparticles based film on conductive Ti plate (NiSe2/Ti) is an efficient and robust electrode to catalyze both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in basic media. Electrochemical experiments show this electrode affords 10 mA cm–2 at HER overpotential of 96 mV and 20 mA cm–2 at OER overpotential of 295 mV with strong durability in 1.0 M KOH. The corresponding two-electrode alkaline water electrolyzer requires a cell voltage of only 1.66 V to achieve 10 mA cm–2 water-splitting current. This development provides us an attractive non-noble-metal catalyst toward overall water splitting applications.