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Coulombic efficiency (CE) measurements in asymmetric Li\u00b0||Cu\u00b0 cells serve as critical evaluative metrics, but the resulting CE values often deviate from expectations based on additive structure alone. Herein, we delve into the design of fluorinated electrolyte additives by combining statistical analysis of Li\u00b0||Cu\u00b0 cycling data with compositional characterization as well as atomistic and chemical simulations. Our results demonstrate that nonafluorobutanesulfonyl fluoride, as an electrolyte additive, induces only a marginal effect on the Aurbach CE values during short\u2010term cycling tests of Li\u00b0||Cu\u00b0 cells. Intriguingly, during extended\u2010cycling, statistical analysis reveals that the same additive exhibits divergent effects in electrolyte families based on bis(trifluoromethanesulfonyl)imide (TFSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) and bis(fluorosulfonyl)imide (FSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) anions. These differences arise from the interplay between the film\u2010forming chemistry of the fluorinated additive and the active involvement of TFSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    and FSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    anions, which collectively modulate the chemical and electrochemical features of the resulting solid\u2010electrolyte interphases (SEI) on Li\u00b0. This work elucidates how additive functionality translates into interphase chemistry and provides a statistically robust framework for screening electrolyte additives for practical lithium metal batteries.\n                  <\/jats:p>","DOI":"10.1002\/anie.9595705","type":"journal-article","created":{"date-parts":[[2026,7,31]],"date-time":"2026-07-31T07:57:41Z","timestamp":1785484661000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Revisiting Coulombic Efficiency Paradigm: Electrolyte Additive Design for Lithium Metal Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Qixin","family":"Wang","sequence":"first","affiliation":[{"name":"Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 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