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However, its strong ionic interlayer bonding of Se layers fundamentally restricts the full potential of this otherwise promising quasi\u2010two\u2010dimensional (2D) material. In this work, we demonstrate chlorine substitution as an effective strategy to introduce van der Waals gaps and modify the electronic structure of the system. Through comprehensive transport and angle\u2010resolved photoemission spectroscopy (ARPES) measurements on Bi\n                    <jats:sub>6<\/jats:sub>\n                    O\n                    <jats:sub>6<\/jats:sub>\n                    Se\n                    <jats:sub>2<\/jats:sub>\n                    Cl\n                    <jats:sub>2<\/jats:sub>\n                    single crystal, an optimal Cl\u2010doping compound, we show that the key electronic features, including indirect bandgap, high electron mobility, and carrier effective mass, are well preserved, while the 2D character of the system is sufficiently enhanced. First\u2010principles calculations attribute this selective tunability to the unique spatial separation between conductive Bi\u2010O layers and dopant Se\/Cl layers, which enables independent optimization of interlayer coupling and intralayer transport. Remarkably, our theoretical calculations combined with experimental observations project a broad bandgap engineering across a wide range (0.8 \u223c 3.5\u00a0eV) within the Bi\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    Se system. Our findings not only expand the application potential of Bi\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    Se\u2010based materials in optoelectronics, nanoelectronics, and fundamental research but also highlight spatial decoupling as a viable strategy for modifying the detailed electronic structure of quasi\u20102D quantum systems.\n                  <\/jats:p>","DOI":"10.1002\/advs.77919","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T18:00:31Z","timestamp":1790532031000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Enhancing Quasi\u2010Two\u2010Dimensional Electronic Structure in Bi\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Se via Chlorine Substitution"],"prefix":"10.1002","author":[{"given":"Yong\u2010Zhen","family":"Jiang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Quantum Functional Materials and ShanghaiTech Laboratory For Topological Physics School of Physical Science and Technology ShanghaiTech University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qi\u2010Xun","family":"Wen","sequence":"additional","affiliation":[{"name":"National Laboratory of Solid State Microstructures Department of Materials Science and Engineering Department of Physics Nanjing University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiang","family":"Xu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Quantum Functional Materials and ShanghaiTech Laboratory For Topological Physics School of Physical Science and Technology ShanghaiTech University  Shanghai 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