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The development of inexpensive, selective, and robust catalysts that enable room temperature conversion will decide the future of this technology. Single\u2010atom catalysts (SACs) with isolated active centers embedded in support have displayed significant promises in catalysis to drive challenging reactions. Herein, high\u2010density Ni single atoms are developed and stabilized on carbon nitride (NiCN) via thermal condensation of preorganized Ni\u2010coordinated melem units. The physicochemical characterization of NiCN with various analytical techniques including HAADF\u2010STEM and X\u2010ray absorption fine structure (XAFS) validate the successful formation of Ni single atoms coordinated to the heptazine\u2010constituted CN network. The presence of uniform catalytic sites improved visible absorption and carrier separation in densely populated NiCN SAC resulting in 100% selective photoconversion of (CH<jats:sub>4<\/jats:sub>) to methanol using H<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub> as an oxidant. The superior catalytic activity can be attributed to the generation of high oxidation (Ni<jats:sup>III<\/jats:sup>\u2550O) sites and selective C\u2500H bond cleavage to generate \u2022CH<jats:sub>3<\/jats:sub> radicals on Ni centers, which can combine with \u2022OH radicals to generate CH<jats:sub>3<\/jats:sub>OH.<\/jats:p>","DOI":"10.1002\/smll.202304574","type":"journal-article","created":{"date-parts":[[2023,11,28]],"date-time":"2023-11-28T00:10:28Z","timestamp":1701130228000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Partial Thermal Condensation Mediated Synthesis of High\u2010Density Nickel Single Atom Sites on Carbon Nitride for Selective Photooxidation of Methane into Methanol"],"prefix":"10.1002","volume":"20","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2804-9298","authenticated-orcid":false,"given":"Pawan","family":"Kumar","sequence":"first","affiliation":[{"name":"Department of Chemical and 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