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In this study, we show that Mn incorporation in carbon nitride\u2010supported single\u2010atom photocatalysts (Mn\n                    <jats:sub>1<\/jats:sub>\n                    @CN\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    ) triggers a regime transition without detectable Mn aggregation. At low\u2010to\u2010intermediate loadings, isolated Mn\u2013N\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    sites are accommodated within a partially delaminated CN\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    framework, promoting productive carrier trapping, oxygen activation, and selective aerobic benzylic C\u2013H oxidation. Above a critical loading, however, Mn incorporation reorganizes the support into a distorted and densified architecture, modifies the Mn coordination environment, and shifts carrier dynamics toward unproductive recombination. Structural, spectroscopic, and computational analyses connect this transition to framework stacking, electronic disorder, and Mn\u2010support coupling. During selective aerobic benzylic C\u2013H oxidation, we show that this regime transition translates into a nonmonotonic activity response, in which additional isolated Mn sites become detrimental once support reorganization overrides the benefit of increased site density. Mechanistic experiments and theory support a photoinduced oxygen activation, with the productive regime enabled by the balance between isolated Mn sites and a favorable CN\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    trap\u2010state landscape. These findings establish single\u2010atom site density as a structural and photophysical design parameter for polymer\u2010supported photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.3256491","type":"journal-article","created":{"date-parts":[[2026,9,24]],"date-time":"2026-09-24T11:15:43Z","timestamp":1790248543000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Site Density Governs Switching Reactivity Regimes During Aerobic C\u2500H Oxidation in Mn Single\u2010Atom Photocatalysts"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-5949-8428","authenticated-orcid":false,"given":"Viktoria","family":"Velichko","sequence":"first","affiliation":[{"name":"Department of Chemistry, Materials and Chemical Engineering \u201cGiulio Natta\u201d Politecnico di Milano  Milano 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