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Strong piezoelectric polarization is essential for sufficient driving force, yet highly polar materials typically suffer from poor conductivity, which limits bulk\u2010to\u2010surface charge transport. Conversely, enhancing conductivity often compromises piezoelectric performance, resulting in a bottleneck in piezocatalysis. Herein, we decouple piezoelectricity and conductivity using atomically dispersed nickel single atoms on amino\u2010functionalized UiO\u201066 (Ni SAs@UiO\u201066\u2010NH\n                    <jats:sub>2<\/jats:sub>\n                    ). Introducing polar amino groups and asymmetric Ni\u2500N coordination significantly enhances the piezoelectric response, increasing the piezoelectric coefficient d\n                    <jats:sub>33<\/jats:sub>\n                    from 48 to 242 pm V\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Simultaneously, hydrogen adsorption at Ni sites under mechanical stress triggers a pressure\u2010induced semiconductor\u2010to\u2010metal transition, creating transient metallic conduction pathways that facilitate efficient electron extraction without sacrificing bulk polarization. As a result, hydrogen adsorption sites shift from framework carbons to Ni centers, yielding near\u2010optimal H\n                    <jats:sup>*<\/jats:sup>\n                    adsorption energetics (\u0394G\n                    <jats:sub>H<\/jats:sub>\n                    <jats:sup>*<\/jats:sup>\n                    approximately 0.12 eV at 100 MPa), and enabling rapid polarization\u2010driven hydrogen evolution. Consequently, the Ni SAs@UiO\u201066\u2010NH\n                    <jats:sub>2<\/jats:sub>\n                    catalyst achieves exceptional hydrogen evolution rate of 1871 \u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    in deionized water and 17\u00a0613 \u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    in methanol\u2010containing media, surpassing reported MOF\u2010based piezocatalysts and competing with leading photo\u2010piezocatalytic and photocatalytic systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.202523489","type":"journal-article","created":{"date-parts":[[2026,3,8]],"date-time":"2026-03-08T11:56:21Z","timestamp":1772970981000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Activating a Metallization Switch for Record Hydrogen Evolution in Single\u2010Atom Modified Polar MOF Piezocatalysts"],"prefix":"10.1002","volume":"38","author":[{"given":"Chongyan","family":"Hao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Silicate Materials for Architectures School of Material Science and Engineering Wuhan University of Technology  Wuhan P. 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