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Rational electrolyte additive design offers an effective route to move beyond single-function regulation toward synergistic multimechanism control. Compared to multicomponent systems, single-molecule additives with multiple functional groups enable integrated control over solvation structure and interfacial chemistry while reducing complexity and cost. Herein, the natural amino acid hydroxyproline (hyp) is introduced as a multifunctional electrolyte additive for simultaneous regulation of the Zn2+ solvation and interfacial chemistry. The \u2212COOH and \u2212OH groups reconstruct the solvation sheath and hydrogen-bond network, while the \u2212NH\u2212 group promotes interfacial adsorption and induces a compact, N-rich interphase that homogenizes Zn2+ flux and suppresses dendrite growth. Benefiting from this cooperative solvation\u2212interphase regulation, stable Zn plating\/stripping is achieved for over 2000 h in Zn\/\/Zn cells, an average coulombic efficiency of 99.79% is maintained over 1500 cycles in Zn\/\/Cu cells, and Zn\/\/LiFePO4 full cells deliver a capacity of 154 mAh g\u22121 over 500 cycles at 0.2 A g\u22121. This work highlights single-molecule, multifunctional electrolyte additive engineering as a rational, scalable strategy for durable, safe aqueous zinc batteries.<\/jats:p>","DOI":"10.1021\/acsami.6c09786","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T08:01:44Z","timestamp":1791446504000},"source":"Crossref","is-referenced-by-count":0,"title":["Single-Molecule Multifunctional Additive Enables Coupled Solvation and Interphase Engineering for Highly Reversible Zinc Anodes"],"prefix":"10.1021","author":[{"given":"Bei","family":"Yan","sequence":"first","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 1H9"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue","family":"Fei","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 1H9"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoyu","family":"Xia","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 1H9"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2901-6228","authenticated-orcid":true,"given":"Yue","family":"Li","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 1H9"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxuan","family":"Wu","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 1H9"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4080-3222","authenticated-orcid":true,"given":"Hao","family":"Zhang","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 1H9"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1978-2976","authenticated-orcid":true,"given":"Ge","family":"Li","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 1H9"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,8]]},"reference":[{"issue":"6","key":"2026100804013870300_cit1","doi-asserted-by":"publisher","first-page":"543","DOI":"10.1038\/s41563-018-0063-z","article-title":"Highly Reversible Zinc Metal Anode for Aqueous Batteries","volume":"17","author":"Wang","year":"2018","journal-title":"Nat. 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