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Te\u2010free BiSbSe\n                    <jats:sub>3<\/jats:sub>\n                    embodies this contradiction: its intrinsically ultralow thermal conductivity makes it promising for medium\u2010temperature thermoelectric applications, while stable\n                    <jats:italic>p<\/jats:italic>\n                    \u2010type transport remains elusive and the optimization limits of both conduction types remain unclear. Here, we reveal that native defects and Sb containing lone\u2010pairs jointly govern its transport behavior. Electron microscopy analysis and first\u2010principles calculations confirm that Se vacancies and cation\u2010on\u2010Se antisite defects possess low formation enthalpies, stabilizing\n                    <jats:italic>n<\/jats:italic>\n                    \u2010type conduction, compensating holes, and pinning the Fermi level away from the valence band maximum. Moreover, strong near\u2010band\u2010edge Sb\u2010Se hybridization softens Sb\u2010dominated low\u2010frequency optical phonons, promoting acoustic\u2010optical coupling and diffuson\u2010like thermal transport at high temperatures. By matching theory and experiment, we identify carrier mobility degradation at high donor concentrations as the main limitation for\n                    <jats:italic>n<\/jats:italic>\n                    \u2010type BiSbSe\n                    <jats:sub>3<\/jats:sub>\n                    . Our calculations predict that eliminating Fermi\u2010level pinning could enable\n                    <jats:italic>p<\/jats:italic>\n                    \u2010type BiSbSe\n                    <jats:sub>3<\/jats:sub>\n                    to achieve an excellent average\n                    <jats:italic>ZT<\/jats:italic>\n                    of \u223c\u00a01.4 over 300\u2010800\u00a0K. These findings not only clarify the long\u2010standing underperformance of ultralow thermal conductivity thermoelectric compounds, but also establish a universal chemical design framework for optimizing Te\u2010free thermoelectrics.\n                  <\/jats:p>","DOI":"10.1002\/adma.74931","type":"journal-article","created":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T05:48:05Z","timestamp":1788932885000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Native Defects\u2010Induced Fermi\u2010Level Pinning and Diffuson\u2010Mediated Thermal Transport in BiSbSe\n                    <sub>3<\/sub>\n                    Thermoelectrics"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-1747-7610","authenticated-orcid":false,"given":"Shulin","family":"Bai","sequence":"first","affiliation":[{"name":"Tianmushan Laboratory Beihang University  Hangzhou China"},{"name":"School of Materials Science and Engineering Beihang University  Beijing China"},{"name":"National Key Laboratory of Artificial Intelligence for Material Science Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2720-5922","authenticated-orcid":false,"given":"Bingchao","family":"Qin","sequence":"additional","affiliation":[{"name":"Tianmushan Laboratory Beihang University  Hangzhou China"},{"name":"School of Materials Science and Engineering Beihang University  Beijing China"},{"name":"State Key Laboratory of Special Materials Surface Engineering School of Materials Science and Engineering Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Da","family":"Wan","sequence":"additional","affiliation":[{"name":"Tianmushan Laboratory Beihang University  Hangzhou China"},{"name":"School of Materials Science and Engineering Beihang University  Beijing China"},{"name":"National Key Laboratory of Artificial Intelligence for Material Science Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4117-8572","authenticated-orcid":false,"given":"Yixuan","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Beihang University  Beijing China"},{"name":"State Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation School of Materials Science and Engineering Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Baocheng","family":"Yuan","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-1475-1242","authenticated-orcid":false,"given":"Tian","family":"Gao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7630-4041","authenticated-orcid":false,"given":"Sining","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenghao","family":"Hou","sequence":"additional","affiliation":[{"name":"Shijiazhuang Key Laboratory of Low Carbon Energy Materials College of Chemical Engineering Shijiazhuang University  Shijiazhuang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi","family":"Wen","sequence":"additional","affiliation":[{"name":"Tianmushan Laboratory Beihang University  Hangzhou China"},{"name":"School of Materials Science and Engineering Beihang University  Beijing China"},{"name":"National Key Laboratory of Artificial Intelligence for Material Science Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1247-4345","authenticated-orcid":false,"given":"Li\u2010Dong","family":"Zhao","sequence":"additional","affiliation":[{"name":"Tianmushan Laboratory Beihang University  Hangzhou China"},{"name":"School of Materials Science and Engineering Beihang University  Beijing China"},{"name":"National Key Laboratory of Artificial Intelligence for Material Science Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,9,8]]},"reference":[{"key":"e_1_2_7_2_1","first-page":"1","article-title":"Designing Advanced Thermoelectrics","volume":"11","author":"Bai S.","year":"2026","journal-title":"Nature Reviews 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