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Addressing these coupled limitations requires a bulk\u2013surface design framework that balances magnetic-frustration-associated cation ordering with nanoscale interphase stability. Here, nominal 1 mol % high-valence, nonmagnetic d0 modifiers (V5+, Hf4+, Ta5+) are used as a chemically defined model series to probe the coupling between magnetic-frustration-associated cation ordering and nanoscale surface\/near-surface interphase architecture. Within this series, 1%Hf-NM64 lowers the apparent frustration index from 9.562 to 7.366 and the refined Li\/Ni mixing from 7.67 to 7.14%, whereas V increases both descriptors and Ta leaves them nearly unchanged. Low-temperature M\u2013H loops further indicate that 1%Hf-NM64 exhibits the weakest hysteretic magnetic irreversibility. Surface\/near-surface characterization reveals modifier-dependent nanoscale interphase architectures, with localized Li2HfO3-rich domains in 1%Hf-NM64 coinciding with the lowest polarization and the best cycling response among the series. Compared with pristine NM64, 1%Hf-NM64 raises the initial 1 C discharge capacity from 136.6 to 159.0 mAh g\u20131 and improves the 500-cycle capacity retention from 69.0 to 73.3%. 3%Hf-NM64 further shows that excessive Hf increases Li2HfO3-related secondary-phase content and apparent Li+ diffusivity but compromises long-term cycling stability. These findings support optimized bulk\u2013surface coupled regulation of magnetic frustration, cation disorder, and interphase architecture as a design principle for Co-free layered oxide cathodes.<\/jats:p>","DOI":"10.1021\/acsami.6c13021","type":"journal-article","created":{"date-parts":[[2026,9,11]],"date-time":"2026-09-11T17:01:51Z","timestamp":1789146111000},"page":"50937-50950","source":"Crossref","is-referenced-by-count":0,"title":["Bulk\u2013Surface Coupled Regulation of Magnetic Frustration and Interphase Architecture in Co-Free LiNi0.6Mn0.4O2 Cathodes"],"prefix":"10.1021","volume":"18","author":[{"given":"Tao","family":"Ye","sequence":"first","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Wei","sequence":"additional","affiliation":[{"name":"Beijing Institute of Technology , , ,","place":["Beijing, China, 100081"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-3441-3614","authenticated-orcid":true,"given":"Zunqiu","family":"Xiao","sequence":"additional","affiliation":[{"name":"China Automotive Battery Research Institute Co., Ltd. , ,","place":["Beijing, China, 101407"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kejia","family":"Xiang","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huaying","family":"Wang","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shaoyu","family":"Mo","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huixian","family":"Jiang","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4860-8774","authenticated-orcid":true,"given":"Junying","family":"Zhang","sequence":"additional","affiliation":[{"name":"Beihang University , , ,","place":["Beijing, China, 100191"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4341-3510","authenticated-orcid":true,"given":"Shitong","family":"Wang","sequence":"additional","affiliation":[{"name":"Beihang University , , ,","place":["Beijing, China, 100191"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0706-0260","authenticated-orcid":true,"given":"Zilong","family":"Tang","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,11]]},"reference":[{"issue":"10","key":"2026102013071969800_cit1","doi-asserted-by":"publisher","first-page":"1215","DOI":"10.1038\/s41560-025-01852-3","article-title":"Zero-strain Mn-rich layered cathode for sustainable and high-energy next-generation batteries","volume":"10","author":"Park","year":"2025","journal-title":"Nat. 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