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This work introduces a conceptually novel strategy of spin\u2010state modulation via interfacial engineering to regulate platinum nanocrystals anchored on atomically dispersed Fe\u2010N\u2010C substrates (Pt\/Fe\n                    <jats:sub>SA<\/jats:sub>\n                    \u2010NC). Based on density functional theory (DFT) predictions, we construct a spin\u2010state\u2010tunable architecture by precisely controlling Pt particle size (2\u20138\u00a0nm), which induces spin\u2010matching effects that effectively mitigate *OH over\u2010binding in pH\u2010dependent ORR path. Mechanistic studies indicate that the synergy between FeN\n                    <jats:sub>4<\/jats:sub>\n                    \u2010mediated metal\u2010support interactions and size\u2010dependent spin polarization facilitates charge transfer, weakening *OH adsorption and promoting its desorption. In alkaline conditions, \u223c2\u00a0nm Pt nanoclusters with moderate spin density achieve a peak power density of 179\u00a0mW cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in Zn\u2010air batteries with 150 h stability. Under acidic media, \u223c8\u00a0nm Pt nanoparticles with low\u2010spin configuration deliver a mass activity of 0.65 A mg\n                    <jats:sub>Pt<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    and a peak power density of 730\u00a0mW cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in proton\u2010exchange membrane fuel cells (PEMFCs), outperforming commercial Pt\/C and retaining 90% activity after 3000 cycles. This finding provides a spin\u2010engineering paradigm for designing advanced electrocatalysts with ultralow Pt loading.\n                  <\/jats:p>","DOI":"10.1002\/anie.202515517","type":"journal-article","created":{"date-parts":[[2025,11,11]],"date-time":"2025-11-11T13:32:49Z","timestamp":1762867969000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Spin\u2010Matching Effect Triggering Enhanced Oxygen Reduction Reaction in Acidic and Alkaline Media"],"prefix":"10.1002","volume":"65","author":[{"given":"Cong\u2010Yi","family":"Du","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering\/Institute of Clean Energy and Materials\/Key Laboratory for Clean Energy and Materials Guangzhou University  Guangzhou 510006 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zi\u2010Qi","family":"Ge","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering\/Institute of Clean Energy and Materials\/Key Laboratory for Clean Energy and Materials Guangzhou University  Guangzhou 510006 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lv\u2010Hao","family":"Ouyang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering\/Institute of Clean Energy and Materials\/Key Laboratory for Clean Energy and Materials Guangzhou University  Guangzhou 510006 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hong\u2010Yi","family":"Xu","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering\/Institute of Clean Energy and Materials\/Key Laboratory for Clean Energy and Materials Guangzhou University  Guangzhou 510006 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hua\u2010Ying","family":"Ma","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering\/Institute of Clean Energy and Materials\/Key Laboratory for Clean Energy and Materials Guangzhou University  Guangzhou 510006 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao\u2010Tong","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering\/Institute of Clean Energy and Materials\/Key Laboratory for Clean Energy and Materials Guangzhou University  Guangzhou 510006 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0727-7809","authenticated-orcid":false,"given":"Zhao\u2010Qing","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering\/Institute of Clean Energy and Materials\/Key Laboratory for Clean Energy and Materials Guangzhou University  Guangzhou 510006 P. R. China"},{"name":"School of Chemistry South China Normal University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,11,11]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560\u2010021\u201000775\u2010z"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c09190"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-25911-x"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D2CS00684G"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2318174121"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010022\u201030702\u2010z"},{"key":"e_1_2_7_7_1","first-page":"0366","volume":"9","author":"Liu F.","year":"2023","journal-title":"Sci. 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