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Despite the difficulty of controlling (pseudo\u2010)polymorphism, the realization of specific (pseudo\u2010)polymorphic phases and associated boundary structures is an efficient route to enhance material performance for energy conversion and electromechanical applications. Here, this work applies the pseudopolymorphic phase (PP) concept to a thermoelectric copper sulfide, Cu<jats:sub>2\u2010<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>S (<jats:italic>x<\/jats:italic> \u2264 0.25), via CuBr<jats:sub>2<\/jats:sub> doping. A peak ZT value of 1.25 is obtained at 773\u00a0K in Cu<jats:sub>1.8<\/jats:sub>S + 3\u00a0wt% CuBr<jats:sub>2<\/jats:sub>, which is 2.3 times higher than that of a pristine Cu<jats:sub>1.8<\/jats:sub>S sample. Atomic\u2010resolution scanning transmission electron microscopy confirms the transformation of pristine Cu<jats:sub>1.8<\/jats:sub>S low digenite into PP\u2010engineered high digenite, as well as the formation of (semi\u2010)coherent interfaces between different PPs, which is expected to enhance phonon scattering. The results demonstrate that PP engineering is an effective approach for achieving improved thermoelectric performance in Cu\u2010S compounds. It is also expected to be useful in other materials.<\/jats:p>","DOI":"10.1002\/adma.202308353","type":"journal-article","created":{"date-parts":[[2023,10,30]],"date-time":"2023-10-30T19:43:20Z","timestamp":1698695000000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["Pseudopolymorphic Phase Engineering for Improved Thermoelectric Performance in Copper Sulfides"],"prefix":"10.1002","volume":"36","author":[{"given":"Tian\u2010Yu","family":"Yang","sequence":"first","affiliation":[{"name":"Faculty of Materials Science and Engineering Kunming University of Science and Technology  Kunming 650093 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shi\u2010Wei","family":"Gu","sequence":"additional","affiliation":[{"name":"Faculty of Materials Science and Engineering Kunming University of Science and Technology  Kunming 650093 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E.","family":"Dunin\u2010Borkowski","sequence":"additional","affiliation":[{"name":"Ernst Ruska\u2010Centre for Microscopy and Spectroscopy with Electrons Forschungszentrum J\u00fclich GmbH  52425 J\u00fclich Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Di","family":"Wu","sequence":"additional","affiliation":[{"name":"Key Laboratory for Macromolecular Science of Shaanxi Province Shaanxi Key Laboratory for Advanced Energy Devices School of Materials Science and Engineering Shaanxi Normal University  Xi'an 710119 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8810-5103","authenticated-orcid":false,"given":"Zhen\u2010Hua","family":"Ge","sequence":"additional","affiliation":[{"name":"Faculty of Materials Science and Engineering Kunming University of Science and Technology  Kunming 650093 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