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Nevertheless, the intrinsic steric constraints imposed by polymeric side chains frequently lead to metastable molecular packing configurations with diminished structural coherence. In this study, a morphological modulation strategy is proposed by adopting a 2D layered hydrotalcite (HDC) nanocrystal to regulate polymeric adsorption dynamics. By leveraging hydroxyl\u2010directed interfacial coordination to HDC matrices, the nanocrystal\u2010integrated BHJ systems manifest a pronounced donor\u2010phase H\u2010aggregation, synergistically coupled with reduced \u03c0\u2010orbital overlap distances and enhanced long\u2010range crystalline ordering. These nanoscale structural advancements collectively engender superior charge transfer kinetics with reduced activation energy barriers and improved charge carrier transport properties. The HDC nanocrystal\u2010blended devices not only achieve a top\u2010notch power conversion efficiency (PCE) of 20.63%, but also shows its applicability across various donor \u2013 acceptor BHJ systems. This work develops a crystal\u2010engineering strategy that concurrently optimizes nanoscale morphology and charge transport networks in OSCs, yielding state\u2010of\u2010the\u2010art device performance through synergistic structural\u2010electronic modulation.<\/jats:p>","DOI":"10.1002\/adma.202508049","type":"journal-article","created":{"date-parts":[[2025,7,2]],"date-time":"2025-07-02T04:11:56Z","timestamp":1751429516000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Regulating Polymeric Adsorption Dynamics via Monolayer\u2010Architected Hydrotalcite Integration for High\u2010Performance Organic Solar Cells"],"prefix":"10.1002","volume":"37","author":[{"given":"Zhenye","family":"Li","sequence":"first","affiliation":[{"name":"College of Mechanical Engineering University of South China  Hengyang 421001 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