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Here, we report a bioinspired strategy for constructing face\u2010to\u2010face supramolecular co\u2010assembled arrays (FF\u2010SCAAs), in which periodic co\u2010facial organization serves as a structural platform for programming electron transport pathways toward enhanced photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production. Inspired by the signal\u2010transport arrays of natural compound eyes, cationic trioxatriangulenium (\n                    <jats:bold>\n                      TOTA\n                      <jats:sup>+<\/jats:sup>\n                    <\/jats:bold>\n                    ) and electron\u2010rich benzophenanthrene derivatives are integrated into highly ordered FF\u2010SCAAs through directional cation\u2010\u03c0 interaction. The resulting FF\u2010SCAAs feature enhanced dipole moments and favorable orbital alignment, enabling extended charge transport channels while intrinsically suppressing electron\u2010hole recombination. On this basis, FF\u2010SCAAs achieve a H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    photosynthesis rate up to 6.46\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    with a solar\u2010to\u2010chemical conversion efficiency of 0.84%. Ultrafast spectroscopic and mechanistic studies demonstrate that the periodic co\u2010facial arrays promote directional excited\u2010state electron migration and selective two\u2010electron oxygen reduction pathways for H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    generation. Furthermore, the in situ generated H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    is fed into a cascade wastewater treatment system and consumed in a downstream Fenton process for efficient degradation of phenolic pollutants.\n                  <\/jats:p>","DOI":"10.1002\/anie.4053685","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T00:27:26Z","timestamp":1790814446000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Bioinspired Face\u2010to\u2010Face Supramolecular Co\u2010Assembled Arrays Enabled by Cation\u2010\u03c0 Interaction With Programmed Electron Transport for Efficient Hydrogen Peroxide Photosynthesis"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1955-7004","authenticated-orcid":false,"given":"Zhao","family":"Gao","sequence":"first","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zeyu","family":"Chen","sequence":"additional","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an China"},{"name":"China Institute of Nuclear Industry Strategy Co., Ltd  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xupeng","family":"Ji","sequence":"additional","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Feiran","family":"Sun","sequence":"additional","affiliation":[{"name":"Aerospace Research Institute of Materials &amp; Processing Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziyou","family":"Wang","sequence":"additional","affiliation":[{"name":"Queen Mary University of London Engineering School Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qi","family":"Wen","sequence":"additional","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zihao","family":"Wang","sequence":"additional","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuncong","family":"Xue","sequence":"additional","affiliation":[{"name":"Organisch\u2010Chemisches Institut Westf\u00e4lische Wilhelms\u2010Universit\u00e4t M\u00fcnster, Corrensstra\u00dfe 36  M\u00fcnster Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yan","family":"Zhao","sequence":"additional","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2159-4181","authenticated-orcid":false,"given":"Wei","family":"Tian","sequence":"additional","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science 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