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Herein, this study innovatively employs the coordination\u2010driven self\u2010assembly of Ni\n                    <jats:sup>2+<\/jats:sup>\n                    ions and perylenetetracarboxylic acid (PTA) to construct a Ni\u2010PTA supramolecular photocatalyst, achieving significantly enhanced photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    evolution performance. Experimental and theoretical results confirm that Ni\n                    <jats:sup>2+<\/jats:sup>\n                    ions are inserted into PTA interlayers via monodentate coordination with carboxyl groups, inducing pronounced charge polarization and substantially augmenting the molecular dipole moment of Ni\u2010PTA. The enhanced dipole establishes a giant internal electric field (IEF) within Ni\u2010PTA, thereby reducing exciton binding energy and increasing charge\u2010separation efficiency by 4.2\u2010fold. Thus, Ni\u2010PTA exhibits excellent and stable photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    evolution, with a rate of 496.7\u00a0\u00b5mol\u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , 3.8 times higher than that of self\u2010assembled PTA supramolecules. Meanwhile, a notable apparent quantum efficiency of 16.5% at 420\u00a0nm is achieved, surpassing most reported supramolecular photocatalysts. Furthermore, the Ni\u2010PTA film sample also shows stable operation with a H\n                    <jats:sub>2<\/jats:sub>\n                    evolution rate of 17.7\u00a0mmol\u00a0m\n                    <jats:sup>\u22122<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , demonstrating promising practical applicability. In summary, this work highlights that metal\u2010coordination engineering enhances the IEF of supramolecular photocatalysts for promoting charge separation, providing a new design strategy for efficient photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/smll.75363","type":"journal-article","created":{"date-parts":[[2026,8,21]],"date-time":"2026-08-21T09:48:42Z","timestamp":1787305722000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Giant Internal Electric Field in Ni\u2010Modified Perylenetetracarboxylic Acid Supramolecule via Metal\u2010Coordination Engineering for Efficient Photocatalytic H\n                    <sub>2<\/sub>\n                    Evolution"],"prefix":"10.1002","volume":"22","author":[{"given":"Peng","family":"Wang","sequence":"first","affiliation":[{"name":"Inertial Confinement Fusion Energy Materials Key Laboratory of Sichuan Province State Key Laboratory of 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