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Herein, we present a strategy to engineer catalyst interfaces by introducing holey defects for highly efficient hydrogen evolution reaction. The holey defects promote uniform dispersion of Pt nanoclusters across the basal planes, rather than the edge\u2010confined deposition observed on pristine ReS\n                    <jats:sub>2<\/jats:sub>\n                    (Pt\u2010hReS\n                    <jats:sub>2<\/jats:sub>\n                    ). Beyond geometric templating, the holey architecture enriches local electron density, stabilizes Pt\u2013S interfacial bridge motifs, tunes the adsorption energy toward near\u2010thermoneutral values, and lowers the water\u2010dissociation barrier. These synergistic effects shift the catalytic regime, moving the rate\u2010determining step from dissociation to desorption, which is revealed in characterizations and density functional theory calculations. Consequently, Pt\u2010hReS\n                    <jats:sub>2<\/jats:sub>\n                    requires only 12\u00a0mV overpotential at 10\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , which outperforms commercial Pt\/C while using substantially less Pt. In an anion\u2010exchange membrane water electrolyzer, a Pt\u2010hReS\n                    <jats:sub>2<\/jats:sub>\n                    cathode achieves 1.77\u00a0V at 0.5 A cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and 1.99\u00a0V at 1.0 A cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , with stable operation exceeding 100\u00a0h. This work establishes holey\u2010defect engineering as a powerful approach for interface optimization, opening new avenues for rational catalyst design in energy\u2010conversion applications.\n                  <\/jats:p>","DOI":"10.1002\/smll.202600032","type":"journal-article","created":{"date-parts":[[2026,3,19]],"date-time":"2026-03-19T09:41:09Z","timestamp":1773913269000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Spatially Extended Interfacial Optimization via Holey\u2010Defect Architectures for Hydrogen Evolution Reaction"],"prefix":"10.1002","volume":"22","author":[{"given":"Chengang","family":"Pei","sequence":"first","affiliation":[{"name":"School of Chemistry and Materials Yangzhou University  Yangzhou P. R. 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