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However, the sluggish kinetics and the difficulty of breaking C\u2500H bond of the Ni\u2010based catalysts limit further application. Herein, three high\u2010entropy layered double hydroxides (HELHs), namely ZnNiFeCoV\u2010HELH, ZnNiFeCoCr\u2010HELH, and ZnNiFeCoAl\u2010HELH (denoted as V\u2010HELH, Cr\u2010HELH, and Al\u2010HELH, respectively), are successfully synthesized. Among them, the V\u2010HELH displays the lowest potential of 1.39\u00a0V at 100\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    compared to Cr\u2010HELH (1.41\u00a0V) and Al\u2010HELH (1.44\u00a0V). After five cycles, the formate yield of V\u2010HELH maintains over 95% of the first cycle with excellent stability. Such outstanding performance surpasses that of most state\u2010of\u2010the\u2010art MOR catalysts reported so far. A series of experiments reveal that the V\u2010HELH exhibits the fastest reaction kinetics and the largest number of active Ni\n                    <jats:sup>3+<\/jats:sup>\n                    species. Further investigations and theoretical calculations prove that the V\u2010HELH shows the strongest methanol adsorption with the lowest energy of \u22123.31\u00a0eV. The introduction of vanadium (V)\u00a0with relatively larger tensile strain optimizes the d\u2500band center of V\u2010HELH (\u22120.54\u00a0eV) and lowers the energy barrier (\u22121.62\u00a0eV) from\n                    <jats:sup>*<\/jats:sup>\n                    CH\n                    <jats:sub>3<\/jats:sub>\n                    O to\n                    <jats:sup>*<\/jats:sup>\n                    CH\n                    <jats:sub>2<\/jats:sub>\n                    O. This work provides new insights for rational design of efficient MOR electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/smll.202411550","type":"journal-article","created":{"date-parts":[[2025,2,16]],"date-time":"2025-02-16T11:26:28Z","timestamp":1739705188000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":24,"title":["High\u2010Entropy Layered Double Hydroxides for Efficient Methanol Electrooxidation"],"prefix":"10.1002","volume":"21","author":[{"given":"Yuying","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yihang","family":"Hu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhaohui","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziheng","family":"Song","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiang","family":"Chen","sequence":"additional","affiliation":[{"name":"Jiangsu Ruijia New Materials Co. Ltd  Rugao Jiangsu Province 226532 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1309-0626","authenticated-orcid":false,"given":"Yu\u2010Fei","family":"Song","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"},{"name":"Quzhou Institute for Innovation in Resource Chemical Engineering  Quzhou Zhejiang Province 324000 P. R. 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