LAUSR

Constructing strong oxide‐support interaction (SOSI) is compelling for modulating the atomic configurations and electronic structures of supported catalysts. Herein, ultrafine iridium oxide nanoclusters (≈1 nm) are anchored on vanadium oxide support (IrO2/V2O5) via SOSI. The as made catalyst, with a unique distorted IrO2 structure, is discovered to significantly boost the performance for pH‐universal oxygen evolution reaction (OER). Based on experimental results and theoretical calculations, the distorted IrO2 active sites with flexible redox states in IrO2/V2O5 server as electrophilic centers balance the adsorption of oxo‐intermediates and effectively facilitate the process of OO coupling, eventually propelling the fast turnover of water oxidation. As a result, IrO2/V2O5 demonstrates not only ultralow overpotentials at 10 mA cm−2 (266 mV, pH = 0; 329 mV, pH = 7; 283 mV, pH = 14) for OER, but also high‐performance overall water electrolysis over a broad pH range, with a potential of mere 1.50 V (pH = 0), 1.65 V (pH = 7) or 1.49 V (pH = 14) at 10 mA cm−2. In addition, SOSI can simultaneously secure the distorted active sites and thus remarkably improving the catalytic stability, making it a promising strategy to develop high‐performance catalytic systems.