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Here, we develop a generalizable colloidal strategy that enables precision synthesis of HEO nanocrystals with compositions spanning quinary to septenary systems. Mechanistic studies reveal that differences in precursor reactivity drive a multistage growth pathway and that cooperative multimetal chemistry\u2500where one metal initiates single-phase nucleation and a vacancy-forming metal promotes cation redistribution during growth\u2500enables homogeneous multication incorporation. The resulting rocksalt HEO nanocrystals can be transformed into spinel phases and exhibit excellent oxygen-evolution reaction activity. Machine-learning-accelerated theoretical analysis and operando characterization identify Co\u2013Co bridge sites on spinel {111} facets as the dominant oxygen-evolution active motifs operating through a lattice oxygen-mediated mechanism. These findings establish guiding principles for controlling nucleation, cation mixing, and active-site formation in compositionally complex oxides, enabling the rational design and data-driven optimization of high-entropy materials.<\/jats:p>","DOI":"10.1021\/jacs.6c07729","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T14:04:13Z","timestamp":1785852253000},"page":"33304-33318","source":"Crossref","is-referenced-by-count":1,"title":["Cooperative\nMultimetal Chemistry Enables Precision\nSynthesis of High-Entropy Oxide Nanocrystal Catalysts"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6961-8018","authenticated-orcid":true,"given":"Baixu","family":"Zhu","sequence":"first","affiliation":[{"name":"Indiana University , , 800 E. Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7543-1751","authenticated-orcid":true,"given":"Liping","family":"Liu","sequence":"additional","affiliation":[{"name":"Virginia Polytechnic Institute and State University , , , ,","place":["Blacksburg, Virginia, United States, 24061"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alex N.","family":"Butrum-Griffith","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. 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Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huayu","family":"Guo","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4721-0350","authenticated-orcid":true,"given":"Nathanael C.","family":"Ramos","sequence":"additional","affiliation":[{"name":"University of Colorado Boulder , , , ,","place":["Boulder, Colorado, United States, 80309"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuanliang","family":"Huang","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu-Hsuan","family":"Hsieh","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shan","family":"Jiang","sequence":"additional","affiliation":[{"name":"Purdue University , , 480 Stadium Mall Drive , , ,","place":["West Lafayette, Indiana, United States, 47907"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9173-3450","authenticated-orcid":true,"given":"Jun","family":"Chen","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Maren","family":"Pink","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaroslav","family":"Losovyj","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. Kirkwood Avenue , , ,","place":["Bloomington, Indiana, United States, 47405"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jeffrey T.","family":"Miller","sequence":"additional","affiliation":[{"name":"Purdue University , , 480 Stadium Mall Drive , , ,","place":["West Lafayette, Indiana, United States, 47907"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8307-5881","authenticated-orcid":true,"given":"Adam","family":"Holewinski","sequence":"additional","affiliation":[{"name":"University of Colorado Boulder , , , ,","place":["Boulder, Colorado, United States, 80309"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruipeng","family":"Li","sequence":"additional","affiliation":[{"name":"Brookhaven National Laboratory , , , ,","place":["Upton, New York, United States, 11973"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7192-5471","authenticated-orcid":true,"given":"Cheng","family":"Wang","sequence":"additional","affiliation":[{"name":"Lawrence Berkeley National Laboratory , , 6 Cyclotron Rd , , ,","place":["Berkeley, California, United States, 94720"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9344-1697","authenticated-orcid":true,"given":"Hongliang","family":"Xin","sequence":"additional","affiliation":[{"name":"Virginia Polytechnic Institute and State University , , , ,","place":["Blacksburg, Virginia, United States, 24061"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6851-2721","authenticated-orcid":true,"given":"Xingchen","family":"Ye","sequence":"additional","affiliation":[{"name":"Indiana University , , 800 E. 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