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Here, we design a bioinspired polydopamine (PDA)\u2010mediated interface to construct a PDA\u2010coated PDI\u2010COOH (PDI\u2010COOH@PDA) photocatalyst. The optimized Pt\/PDI\u2010COOH@PDA achieves a hydrogen evolution rate of 18.8\u00a0mmol\u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    and an apparent quantum yield (AQY) of 2.1% at 420\u00a0nm, representing a 3.5\u2010fold enhancement over Pt\/PDI\u2010COOH. Rather than acting as a passive coating, PDA functions as an active interfacial regulator by creating a favorable interfacial reaction microenvironment, anchoring the Pt cocatalyst, and stabilizing the supramolecular framework. The hydrophilic PDA surface promotes water enrichment, while PDA\u2010induced interfacial polarization regulates photogenerated charge dynamics, favoring charge separation and utilization. Meanwhile, the catechol and amino groups of PDA facilitate Pt anchoring, and hydrogen bonding and \u03c0\u2013\u03c0 stacking interactions between PDA and PDI\u2010COOH reinforce the supramolecular framework. These coupled effects enable efficient and durable hydrogen evolution, highlighting PDA\u2010mediated interfacial engineering as an effective strategy for advancing PDI\u2010based supramolecular photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/smtd.71051","type":"journal-article","created":{"date-parts":[[2026,9,22]],"date-time":"2026-09-22T07:08:07Z","timestamp":1790060887000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Polydopamine\u2010Mediated Interfacial Engineering of Perylene Diimide Organic Semiconductors for Photocatalytic Hydrogen Evolution"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-8415-2759","authenticated-orcid":false,"given":"Li","family":"Yang","sequence":"first","affiliation":[{"name":"School of Chemical &amp; Environmental Engineering China University of Mining and Technology (Beijing)  Beijing 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