Exploring high-active catalyst for oxygen evolution reaction (OER) is paramount for efficient and eco-friendly conversion of renewable electricity to hydrogen fuels. In this study, we report a new strategy to significantly enhance the OER activity of NiSe nanochains via growth of uniformly vertical FeOOH ultrathin nanoneedles on the surface. The as-prepared catalyst demonstrates splendid OER performance with a low overpotential of 249.0 mV for driving a current density of 10 mA cm, yielding a small Tafel slope of 46 mV dec. After continuous operation of 10 h, a tiny degeneration of 4.0% is afforded, evidencing the excellent durability of the catalyst. On the basis of electrochemical measurement together with theoretical analysis, we attribute the boosted OER kinetics to the synergistic effect of electron, geometry and interface, concretely, two main reasons should be emphasized: 1) the complementary adsorption/desorption nature of nickel and iron leads to optimized Gibbs free energy; 2) redistribution of localized π-symmetry electrons at the interface endows the favorable adsorption/desorption for the oxygenated species. We anticipate that our work would push boundaries for the fabrication of high-performance transition metal- and selenium-based electrocatalysts.