obstacles: the slow kinetics, the short operation lifespan of electrodes, and the high price of noble-metal catalysts. [2] Thus, developing low-cost, high-efficiency and robust electrocatalysts for overall water splitting is exceptionally urgent. [3] At present, transition metal compounds (TMCs), with earth-abundant nature, versatile redox valence, and unsaturated transition metal sites, have been widely investigated for overall water splitting. However, the intrinsically poor activity and unsatisfied stability greatly hinder their practical applications. [4] Tuning electronic structure is regarded to be an efficient strategy to enhance the activity of electrocatalysts. Strain engineering is one of the promising routes to manipulate the electronic structure by modifying the distances of atoms and in turn favoring the catalytic activity improvement. [5] Previous studies have suggested that by introducing only 1% strain, the d band center can be shifted by ≈0.1 eV, leading to the enhanced binding strengthen between catalytically active sites and surface adsorbates. [5a,6] At present, lattice mismatch, substrate induced and heteroatom substitution are three common strategies for introducing lattice strain. [7] Lattice Developing highly efficient non-noble-metal electrocatalysts for water splitting is crucial for the development of clean and reversible hydrogen energy. Introducing lattice strain is an effective strategy to develop efficient electrocatalysts. However, lattice strain is typically co-created with heterostructure, vacancy, or substrate effects, which complicate the identification of the strainactivity correlation. Herein, a series of lattice-strained homogeneous NiS x Se 1−x nanosheets@nanorods hybrids are designed and synthesized by a facile strategy. The NiS 0.5 Se 0.5 with ≈2.7% lattice strain exhibits outstanding activity for hydrogen and oxygen evolution reaction (HER/OER), affording low overpotentials of 70 and 257 mV at 10 mA cm −2 , respectively, as well as excellent long-term durability even at a large current density of 100 mA cm −2 (300 h), significantly superior to other benchmarks and precious-metal catalysts. Experimental and theoretical calculation results reveal that the generated lattice strain decreases the metal d-orbital overlap, leading to a narrower bandwidth and a closer d-band center toward the Fermi level. Thus, NiS 0.5 Se 0.5 possesses favorable H* adsorption kinetics for HER and lower energy barriers for OER. This work provides a new insight to regulate the lattice strain of advanced catalyst materials and further improve the performance of energy conversion technologies.