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The charge transport through peptides can be effectively modulated via intrinsic composition, structure, and, most notably, interfacial engineering. However, achieving specific electrical properties, such as solid\u2010state rectification, remains a challenge in peptide\u2010based bioelectronics. To fill this gap, a solid\u2010state heterojunction is designed based on the uniform and densely\u2010packed bilayers composed of peptide and quantum dots (QDs) self\u2010assembled monolayer. The presence of a QDs monolayer markedly regulates the rectification and static dielectric constant (\n                    <jats:italic>\n                      \u025b\n                      <jats:sub>r<\/jats:sub>\n                    <\/jats:italic>\n                    ) of the peptide\u2010based heterojunctions. The solid\u2010state rectification ratio of peptide junctions can be raised up to \u224810\n                    <jats:sup>3<\/jats:sup>\n                    , and the\n                    <jats:italic>\n                      \u025b\n                      <jats:sub>r<\/jats:sub>\n                    <\/jats:italic>\n                    increases by a factor of 3. Both the rectification ratio and\n                    <jats:italic>\n                      \u025b\n                      <jats:sub>r<\/jats:sub>\n                    <\/jats:italic>\n                    of peptide\/QDs heterojunctions increase with enhanced non\u2010covalent interactions between peptide side chains and QDs. The interfacial interaction modulates the coupling across the interface, influencing the energy level alignment at the peptide\/QDs interface. This leads to distinct charge transport pathways under opposite bias polarities, thus achieving the regulation of rectification. These findings suggest that strengthening interfacial interactions can increase both rectification and\n                    <jats:italic>\n                      \u025b\n                      <jats:sub>r<\/jats:sub>\n                    <\/jats:italic>\n                    . This deepens the understanding of interface\u2010regulated molecular charge transport and offers a theoretical framework for optimizing the biomolecular solid\u2010state rectification.\n                  <\/jats:p>","DOI":"10.1002\/smll.202500346","type":"journal-article","created":{"date-parts":[[2025,5,27]],"date-time":"2025-05-27T08:51:22Z","timestamp":1748335882000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Interface Regulated Solid\u2010State Rectification of Peptide via Quantum Dots Self\u2010Assembly Monolayer"],"prefix":"10.1002","volume":"21","author":[{"given":"Ying","family":"Wang","sequence":"first","affiliation":[{"name":"College of Chemistry and Molecular Sciences Wuhan University  299 Bayi Road Wuhan Hubei 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunxia","family":"Feng","sequence":"additional","affiliation":[{"name":"Department of Materials Science and 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