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Herein, uniformly dispersed and favorable biosafety profile graphitic carbon nitride quantum dots immobilized with Fe\u2010N<jats:sub>4<\/jats:sub> moieties modulated by axial O atom (denoted as O\u2010Fe\u2010N<jats:sub>4<\/jats:sub>) are developed for converting H<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub> into <jats:sup>1<\/jats:sup>O<jats:sub>2<\/jats:sub> via Russell reaction, without introducing external energy. Notably, O\u2010Fe\u2010N<jats:sub>4<\/jats:sub> performs two interconnected catalytic properties: glutathione oxidase\u2010mimic activity to provide substrate for subsequent <jats:sup>1<\/jats:sup>O<jats:sub>2<\/jats:sub> generation, avoiding the blunting anticancer efficacy by glutathione. The O\u2010Fe\u2010N<jats:sub>4<\/jats:sub> catalyst demonstrates a specific activity of 79.58 U mg<jats:sup>\u22121<\/jats:sup> at pH 6.2, outperforming the most reported Fe\u2010N<jats:sub>4<\/jats:sub> catalysts. Density functional theory calculations demonstrate that the axial O atom can effectively modulate the relative position and electron affinity between Fe and N, lowering the activation energy, strengthening the selectivity, and thus facilitating the Russell\u2010type reaction. The gratifying enzymatic activity stemming from the well\u2010defined Fe\u2010N\/O structure can inhibit tumor proliferation by efficiently downregulating glutathione peroxidase 4 activity and inducing lipid peroxidation. Altogether, the O\u2010Fe\u2010N<jats:sub>4<\/jats:sub> catalyst not only represents an efficient platform for self\u2010cascaded catalysis to address the limitations of <jats:sup>1<\/jats:sup>O<jats:sub>2<\/jats:sub>\u2010involved cancer treatment but also provides a paradigm to enhance the performance of the Fe\u2010N<jats:sub>4<\/jats:sub> catalyst.<\/jats:p>","DOI":"10.1002\/advs.202307254","type":"journal-article","created":{"date-parts":[[2024,7,1]],"date-time":"2024-07-01T05:15:42Z","timestamp":1719810942000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Axial O Atom\u2010Modulated Fe(III)\u2010N<sub>4<\/sub> Sites for Enhanced Cascade Catalytic <sup>1<\/sup>O<sub>2<\/sub>\u2010Induced Tumor Therapy"],"prefix":"10.1002","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1324-0700","authenticated-orcid":false,"given":"Hongji","family":"Liu","sequence":"first","affiliation":[{"name":"High Magnetic Field Laboratory Hefei Institutes of Physical Science Chinese Academy of Sciences  Hefei Anhui 230031 P. 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