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While mixed Cl/Br or Br/I alloy compositions can be formed with no miscibility gaps, this is precluded for mixed Cl/I compositions, due to the large difference in Cl                     <jats:sup>−</jats:sup>                     and I                     <jats:sup>−</jats:sup>                     ionic radii. Here, perovskite‐chalcohalide CsPbCl                     <jats:sub>3</jats:sub>                     –Pb                     <jats:sub>4</jats:sub>                     S                     <jats:sub>3</jats:sub>                     Cl                     <jats:sub>2</jats:sub>                     nanocrystal heterostructures are exploited to study the Cl→I exchange and to isolate new types of intermediate structures. The epitaxial interface between the Pb                     <jats:sub>4</jats:sub>                     S                     <jats:sub>3</jats:sub>                     Cl                     <jats:sub>2</jats:sub>                     chalcohalide and the CsPbCl                     <jats:sub>3</jats:sub>                     perovskite significantly influences the intermediate stages of halide exchange in the perovskite domain, leading to coexisting CsPbCl                     <jats:sub>3</jats:sub>                     and CsPbI                     <jats:sub>3</jats:sub>                     domains, thereby delivering segmented CsPbI                     <jats:sub>3</jats:sub>                     –CsPbCl                     <jats:sub>3</jats:sub>                     –Pb                     <jats:sub>4</jats:sub>                     S                     <jats:sub>3</jats:sub>                     Cl                     <jats:sub>2</jats:sub>                     , energetically favorable heterostructures, with partial I‐alloying of the CsPbCl                     <jats:sub>3</jats:sub>                     domain and at the perovskite–chalcohalide interface. The I:CsPbCl                     <jats:sub>3</jats:sub>                     domain between CsPbI                     <jats:sub>3</jats:sub>                     and Pb                     <jats:sub>4</jats:sub>                     S                     <jats:sub>3</jats:sub>                     Cl                     <jats:sub>2</jats:sub>                     enables a gradual lattice expansion across the heterostructure. This design accommodates interfacial strain, with a 5.6% mismatch at the CsPbCl                     <jats:sub>3</jats:sub>                     –CsPbI                     <jats:sub>3</jats:sub>                     interface and a 3.4% mismatch at the perovskite–chalcohalide interface. Full halide exchange leads to CsPbI                     <jats:sub>3</jats:sub>                     –Pb                     <jats:sub>4</jats:sub>                     S                     <jats:sub>3</jats:sub>                     Cl                     <jats:sub>2</jats:sub>                     heterostructures. Both in intermediate and fully exchanged heterostructures, the CsPbI                     <jats:sub>3</jats:sub>                     domain is emissive. In the intermediate structures, the band alignment between the two perovskite domains is type‐I, with the carriers photogenerated in the CsPbCl                     <jats:sub>3</jats:sub>                     domain quickly transferring to the CsPbI                     <jats:sub>3</jats:sub>                     domain, where they can recombine radiatively.                   </jats:p>"],"publicationDate":"2025-11-06","publisher":"Wiley","embargoEndDate":"2025-12-01","sources":["Crossref","Adv Mater"],"formats":null,"contributors":null,"coverages":null,"bestAccessRight":{"code":"c_abf2","label":"OPEN","scheme":"http://vocabularies.coar-repositories.org/documentation/access_rights/"},"container":{"name":"Advanced 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