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Here, we employ in situ Kelvin probe force microscopy (KPFM) to reveal unexpected electron accumulation on nonpolar {010} facets in wurtzite ZnO platelets (N\u2010ZnO), which represents a dynamic \u201celectron spillover\u201d process beyond static facet confinement. Crucially, femtosecond transient absorption (fs\u2010TA) spectroscopy directly captures interfacial electron transfer from polar Zn\u2010terminated (0001) facets (Zn\u2010ZnO) to N\u2010ZnO with a lifetime of 60.82\u00a0ps. However, electrons spilling over from Zn\u2010ZnO to N\u2010ZnO recombine with the photogenerated holes inherent to N\u2010ZnO, thereby turning it into a recombination center. Guided by this insight, we construct a dual\u2010cocatalyst architecture (AuZnOCo): Au is selectively anchored on N\u2010ZnO and Zn\u2010ZnO to extract electrons, and Co\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    is deposited on O\u2010terminated (000) facets (O\u2010ZnO) to trap holes. The loading of dual cocatalysts promotes charge separation and suppresses this electron spillover\u2011induced recombination. Quantitative analysis reveals \u22483739 holes localized on O\u2010ZnO, \u22481771 electrons on Zn\u2010ZnO, and \u2248812 electrons on N\u2010ZnO in AuZnOCo, while the electron diffusion length (\n                    <jats:italic>L<\/jats:italic>\n                    ) increases from 81.41 to 121.77\u00a0nm. This work deciphers the spatiotemporal resolution of charge\u2010carrier dynamics, offering a blueprint for rationally engineering anisotropic photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.3894018","type":"journal-article","created":{"date-parts":[[2026,7,6]],"date-time":"2026-07-06T08:26:06Z","timestamp":1783326366000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Spatiotemporal Mapping of Field\u2010Driven Electron Spillover across ZnO Facets"],"prefix":"10.1002","volume":"65","author":[{"given":"Zheng","family":"Meng","sequence":"first","affiliation":[{"name":"Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry China University of Geosciences, 68 Jincheng Street  Wuhan P. R. 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