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Nevertheless, the complex local chemical environments in HEMs induce significant differences in intermediate adsorption\/desorption at metal active sites and complicate photoexcited electron transfer. Herein, we propose a strategy of incorporating heterogeneous transition metal Zn into a high\u2010entropy oxide (HEO) lattice to precisely tune the spin state of Ni\n                    <jats:sup>2+<\/jats:sup>\n                    . Since the spin\u2010state transition of Ni\n                    <jats:sup>2+<\/jats:sup>\n                    does not involve electron transfer from t\n                    <jats:sub>2g<\/jats:sub>\n                    to e\n                    <jats:sub>g<\/jats:sub>\n                    orbitals, but rather only involves electron redistribution within e\n                    <jats:sub>g<\/jats:sub>\n                    manifold, its electronic structure is particularly sensitive to lattice distortion\u2010induced variations in crystal\u2010field strength, thereby enabling selective regulation of Ni\n                    <jats:sup>2+<\/jats:sup>\n                    from low\u2010spin to high\u2010spin. Field\u2010dependent magnetization measurements and x\u2010ray absorption spectroscopy confirm that Zn incorporation effectively modulates the spin state of Ni\n                    <jats:sup>2+<\/jats:sup>\n                    . Density functional theory calculations and femtosecond transient absorption spectroscopy reveal that high\u2010spin Ni\n                    <jats:sup>2+<\/jats:sup>\n                    exhibits an upshifted\n                    <jats:italic>d<\/jats:italic>\n                    \u2010band center and pronounced spin polarization, which synergistically optimize both *H adsorption and photogenerated charge carrier separation efficiency. Consequently, 0.75%FeCoNi\n                    <jats:sub>0.3<\/jats:sub>\n                    MnZn\u2013HEO\/Cd\n                    <jats:sub>3<\/jats:sub>\n                    (C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>3<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    (0.75%Ni\n                    <jats:sub>0.3<\/jats:sub>\n                    Zn\u2013HEO\/CdTMT) exhibits a prominent PHE rate of 47.53\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    . This work opens new paradigms for the rational design of spin\u2010directed multi\u2010component HEMs.\n                  <\/jats:p>","DOI":"10.1002\/adma.74778","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T03:54:02Z","timestamp":1787370842000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Spin Engineering of Ni\u2010Based High\u2010Entropy Oxide Cocatalyst: Synchronously Optimizing Intermediate Adsorption and Charge Carrier Separation for Photocatalytic Hydrogen Evolution"],"prefix":"10.1002","volume":"38","author":[{"given":"Kangning","family":"Wang","sequence":"first","affiliation":[{"name":"Key Laboratory of Green and Precise Synthetic Chemistry and Applications Ministry of Education Huaibei Key Laboratory of Low\u2010Carbon Conversion of Small\u2010Molecule Resources School of Chemistry and Chemical Engineering Huaibei Normal University  Huaibei P. R. China"},{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials &amp; CAS\u2010HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry &amp; University of Chinese Academy of Sciences Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0056-5653","authenticated-orcid":false,"given":"Kai","family":"Dai","sequence":"additional","affiliation":[{"name":"Key Laboratory of Green and Precise Synthetic Chemistry and Applications Ministry of Education Huaibei Key Laboratory of Low\u2010Carbon Conversion of Small\u2010Molecule Resources School of Chemistry and Chemical Engineering Huaibei Normal University  Huaibei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6689-8923","authenticated-orcid":false,"given":"Yong","family":"Chen","sequence":"additional","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials &amp; CAS\u2010HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry &amp; University of Chinese Academy of Sciences Chinese Academy of Sciences  Beijing P. R. 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