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Herein, we report the supramolecular assembly of gold nanoclusters (Au NCs) protected by a custom-designed ligand, 1-(4-carboxyphenyl)-5-mercapto-1H-tetrazole (CPMT), which achieved the aforementioned outstanding performance. The CPMT ligand not only stabilized the Au NCs through bidentate Au\u2013S\/Au\u2013N coordination, but also induced supramolecular assembly via intermolecular \u03c0\u2013\u03c0 interactions and hydrogen bonding. The obtained self-assembled CPMT-Au NCs exhibited an exceptionally long ECL lifetime of 60.48 \u03bcs, since their rigid spherical superstructure effectively minimized interfacial nonradiative decay, leading to an intrinsically prolonged excited-state lifetime, and passivated the emissive cores against oxygen quenching, preserving the long-lived emission under ambient conditions. Concurrently, the assembly showcased a remarkably large Stokes shift of 490 nm, which virtually eliminated self-absorption even in the solid state. The assembled CPMT-Au NCs displayed dramatically enhanced ECL efficiency of 353.37%, a 15-fold enhancement over their nonassembled counterparts, attributable to the synergistic suppression of interfacial energy dissipation and self-absorption as well as the improved electrochemical excitation. Additionally, a sensitive sensing platform for carboxylesterase (CE) activity related to early hepatocellular carcinoma was developed with a detection limit of 1.98 \u00d7 10\u20137 U\/L. Therefore, this work establishes supramolecular assembly driven by ligand engineering as a rational platform for regulating the excited-state properties of metal nanoclusters, opening new avenues for high-performance ECL emitters in lifetime-based sensing, high-brightness devices, and multiplexed bioassays.<\/jats:p>","DOI":"10.1021\/acs.analchem.6c03019","type":"journal-article","created":{"date-parts":[[2026,7,16]],"date-time":"2026-07-16T07:10:07Z","timestamp":1784185807000},"page":"21793-21802","source":"Crossref","is-referenced-by-count":1,"title":["Ligand-Driven\nSupramolecular Assembly of Gold Nanoclusters\nwith Ultralong Lifetime and Large Stokes Shift for High-Efficiency\nElectrochemiluminescence"],"prefix":"10.1021","volume":"98","author":[{"given":"Mingyang","family":"Xia","sequence":"first","affiliation":[{"name":"Henan University , , ,","place":["Kaifeng, China, 475001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongyan","family":"Liu","sequence":"additional","affiliation":[{"name":"Henan University , , ,","place":["Kaifeng, China, 475001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Congrui","family":"Zhang","sequence":"additional","affiliation":[{"name":"Henan University , , ,","place":["Kaifeng, China, 475001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xianwei","family":"Chen","sequence":"additional","affiliation":[{"name":"Henan University , , ,","place":["Kaifeng, China, 475001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Tang","sequence":"additional","affiliation":[{"name":"Henan University , , ,","place":["Kaifeng, China, 475001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8203-245X","authenticated-orcid":true,"given":"Yanmei","family":"Zhou","sequence":"additional","affiliation":[{"name":"Henan University , , ,","place":["Kaifeng, China, 475001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5955-3169","authenticated-orcid":true,"given":"Yamin","family":"Nie","sequence":"additional","affiliation":[{"name":"Henan University , , ,","place":["Kaifeng, China, 475001"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,16]]},"reference":[{"key":"2026072808071095200_cit1","doi-asserted-by":"publisher","first-page":"217098","DOI":"10.1016\/j.ccr.2025.217098","article-title":"Organic Frameworks-Based\nElectrochemiluminescence Sensors for Point-of-Care Testing","volume":"546","author":"Zhang","year":"2026","journal-title":"Coord. 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