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Extensive electrolyte engineering has been pursued, yet the intrinsic structural constraints of cathodes remain largely overlooked. Here, we apply a systematic half\u2010cell decoupling strategy across 36 electrolyte formulations to identify the precise rate\u2010determining step (RDS) in graphite (Gr), layered NCM811, and olivine LFP electrodes. Our results show that LT anodic delithiation maintains near\u2010theoretical lithium utilization (\u2248100%), confirming that full\u2010cell failure originates predominantly from the cathode. Notably, even with highly optimized electrolytes, cathodes exhibit a persistent capacity retention ceiling of 82%\u201385% for NCM811 and only 38%\u201348% for LFP. Distribution of capacitive times (DCT) analysis reveals that cathode performance is predominantly dominated by severely hindered bulk Li\n                    <jats:sup>+<\/jats:sup>\n                    diffusion: the solid\u2010state diffusion time in LFP surges from 16.2 min at RT to 104 h at \u221230\u00b0C. These findings conclusively establish sluggish bulk Li\n                    <jats:sup>+<\/jats:sup>\n                    diffusion as the primary kinetic bottleneck, urging a paradigm shift from electrolyte\u2010centric strategies toward intrinsic cathode structural engineering.\n                  <\/jats:p>","DOI":"10.1002\/smll.76123","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T12:42:36Z","timestamp":1791463356000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cathode Bulk Diffusion Dictates Low\u2010Temperature Performance in Li\u2010Ion Batteries: Beyond Electrolyte Engineering"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-5635-2645","authenticated-orcid":false,"given":"Xue","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Materials Science and Engineering Hainan University  Haikou People's Republic of China"},{"name":"Institute of Nuclear and New Energy Technology Tsinghua University  Beijing People's Republic of China"},{"name":"School of Information and Communication Engineering Hainan University  Haikou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4841-4918","authenticated-orcid":false,"given":"Leqiong","family":"Xie","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Materials Science and Engineering Hainan University  Haikou People's Republic of China"},{"name":"Institute of Nuclear and New Energy Technology Tsinghua University  Beijing People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingqiang","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Tropic Ocean 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7146-4097","authenticated-orcid":false,"given":"Xiangming","family":"He","sequence":"additional","affiliation":[{"name":"Institute of Nuclear and New Energy Technology Tsinghua University  Beijing People's Republic of 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