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Here, we report liquid-crystalline polymers (LCPs) as nanoporous films that regulate Li+ flux through directionally aligned ion pathways. Crosslinked LCP films form aligned nanoporous channels (\u223c19 nm), while tethered poly(ethylene glycol) (PEG) chains lining the pore walls provide coordination sites that facilitate Li+ transport. Vertically aligned PEG-LCP films establish through-plane ion pathways, reducing effective tortuosity by \u223c2.5-fold compared with planar alignment despite comparable pore architectures. This structural anisotropy leads to high ionic conductivity (1.77 mS cm\u20131) and a reduced activation energy (0.12 eV) for Li+ migration in carbonate-based electrolytes. The resulting uniform Li+ flux suppresses dendritic and porous Li growth, enabling more uniform Li deposition and mitigating excessive interphase formation. Li metal cells employing vertically aligned PEG-LCP films exhibit stable cycling under fast-charging conditions (4 C) with LiNi0.8Co0.1Mn0.1O2, retaining 94% of the capacity after 100 cycles with an average Coulombic efficiency of 99.86%. This work demonstrates that liquid-crystalline alignment can be leveraged to engineer low-tortuosity ion transport pathways, offering a design principle for fast-charging Li metal batteries.<\/jats:p>","DOI":"10.1021\/acsnano.6c09591","type":"journal-article","created":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T21:02:02Z","timestamp":1790629322000},"page":"27158-27171","source":"Crossref","is-referenced-by-count":0,"title":["Directional Li+ Flux Control via Liquid-Crystalline\nPolymer Separators for Fast-Charging Lithium Metal Batteries"],"prefix":"10.1021","volume":"20","author":[{"given":"Geunjung","family":"Lee","sequence":"first","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6051-9427","authenticated-orcid":true,"given":"Rak Hyeon","family":"Choi","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Geonhyeong","family":"Park","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juri","family":"Kim","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Younwoo","family":"Kim","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hye Ryung","family":"Byon","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9383-8958","authenticated-orcid":true,"given":"Dong Ki","family":"Yoon","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]},{"name":"Gwangju Institute of Science and Technology , , ,","place":["Gwangju, Republic of Korea, 61005"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,28]]},"reference":[{"key":"2026101310083100800_cit1","doi-asserted-by":"publisher","first-page":"194","DOI":"10.1038\/nnano.2017.16","article-title":"Reviving the lithium metal anode for high-energy batteries","volume":"12","author":"Lin","year":"2017","journal-title":"Nat. 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