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Ammonia\u2010to\u2010hydrogen conversion is a demanding example, because Ru\u2010free catalysts must overcome the intrinsically sluggish kinetics of ammonia decomposition. Here, we report a catalyst design that couples precursor\u2010level cation mixing and active\u2010site dispersion with charge\u2010transfer engineering of Ni to address this challenge. Density functional theory calculations identify Cr as the most effective electron\u2010donating promoter for Ni among metal cations incorporable into the precursor framework. Guided by this prediction, we construct a NiCrAl reduced mixed\u2010metal oxide catalyst in which atomically mixed precursors stabilize highly dispersed Ni species, while Cr\u2010to\u2010Ni charge transfer generates electron\u2010rich Ni active sites. Multiscale spectroscopic analyses verify this electronic modulation, and combined theoretical and in situ mechanistic analyses indicate that electron\u2010rich Ni favors NH\n                    <jats:sub>3<\/jats:sub>\n                    adsorption in a reaction\u2010relevant Lewis\u2010acid configuration, favorably modifies the dehydrogenation energetics, and weakens N\n                    <jats:sub>2<\/jats:sub>\n                    binding to facilitate product desorption. NiCrAl\u2010RMMO reaches 95.5% NH\n                    <jats:sub>3<\/jats:sub>\n                    conversion at 550\u00b0C and 22.83\u00a0mmol H\n                    <jats:sub>2<\/jats:sub>\n                    g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    min\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 500\u00b0C, with stable operation over 100\u00a0h. More broadly, this work establishes charge\u2010transfer engineering in LDH\u2010derived mixed\u2010metal nanostructures as a general strategy for designing high\u2010performance, Ru\u2010free catalysts for ammonia\u2010to\u2010hydrogen conversion.\n                  <\/jats:p>","DOI":"10.1002\/advs.78184","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T05:25:36Z","timestamp":1791350736000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Electron\u2010Rich Nickel Enabled by Charge Transfer in Multimetal Nanostructures for Efficient Ammonia\u2010to\u2010Hydrogen Conversion"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-0027-8226","authenticated-orcid":false,"given":"Donghyeok","family":"Kim","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST)  Ulsan 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Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-5729-180X","authenticated-orcid":false,"given":"Jongkyoung","family":"Kim","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST)  Ulsan Republic of Korea"},{"name":"UNIST InnoCORE hydro*studio Ulsan National Institute of Science and Technology (UNIST)  Ulsan Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-3220-9696","authenticated-orcid":false,"given":"Myeung\u2010Jin","family":"Lee","sequence":"additional","affiliation":[{"name":"Ulsan Technology Application Division Korea Institute of Industrial Technology (KITECH)  Ulsan Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bora","family":"Jeong","sequence":"additional","affiliation":[{"name":"Ulsan Technology Application Division Korea 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