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The prospect of enhancing stability by substituting organic transport layers with suitable inorganic compounds, particularly Cu\u2010based inorganic hole\u2010transport materials (HTMs), holds promise due to their high valence band maximum (VBM) aligning with perovskite characteristics. This review assesses the advantages and disadvantages of these five types of Cu\u2010based HTMs. Although Cu\u2010based binary oxides and chalcogenides face narrow bandgap issues, the \u201cchemical modulation of the valence band\u201d (CMVB) strategy has successfully broadened the bandgap for Cu\u2010based ternary oxides and chalcogenides. However, Cu\u2010based ternary oxides encounter challenges with low mobility, and Cu\u2010based ternary chalcogenides face mismatches in VBM alignment with perovskites. Cu\u2010based binary halides, especially CuI, exhibit excellent properties such as wider bandgap, high mobility, and defect tolerance, but their stability remains a concern. These limitations of single anion compounds are insightfully discussed, offering solutions from the perspective of practical application. Future research can focus on Cu\u2010based composite anion compounds, which merge the advantages of single anion compounds. Additionally, mixed\u2010cation chalcogenides such as Cu\n                    <jats:sub>x<\/jats:sub>\n                    M\n                    <jats:sub>1\u2212x<\/jats:sub>\n                    S enable the customization of HTM properties by selecting and adjusting the proportions of cation M.\n                  <\/jats:p>","DOI":"10.1002\/adma.202402412","type":"journal-article","created":{"date-parts":[[2024,5,20]],"date-time":"2024-05-20T07:54:31Z","timestamp":1716191671000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":26,"title":["Critical Review of Cu\u2010Based Hole Transport Materials for Perovskite Solar Cells: From Theoretical Insights to Experimental Validation"],"prefix":"10.1002","volume":"36","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6216-4604","authenticated-orcid":false,"given":"Qingde","family":"Sun","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Nanyang 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