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Therefore, it is pivotal yet significantly challenging to effectively control Li nucleation and deposition in LMBs. Here, we engineer a Janus Ag nanoskin\u2010armored polyimide (Ag@PI\/PI) bilayer separator by in situ growth Ag nanoparticles on the surface of PI nanofiber and integrating a high\u2010strength PI nanofiber membrane as the dorsal substrate. Specifically, the Ag nanoskin acts as a three\u2010dimensional lithiophilic host to seize Li and induce sequential Li nucleation, thereby preventing Li dendrite formation. As a result, the Ag@PI\/PI\u2010Li||Cu cell exhibits a low overpotential of 31.0\u00a0mV, high Coulombic efficiency of 98.9%, and prolonged Sand's time of 26.3\u00a0h. Significantly, the Ag@PI\/PI separator delivers a high Li\n                    <jats:sup>+<\/jats:sup>\n                    transference number (0.70) and exceptional cycling stability (1600\u00a0h) in a Li||Li cell. Moreover, the Ag@PI\/PI\u2010based Li||NCM523 cell achieves a remarkable specific capacity of 108.32 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 5 C while retaining a satisfying capacity retention of 88.7% at 1 C. These results underscore the viability of this universal and efficient Ag nanoskin\u2010armored strategy for high\u2010security LMBs applications.\n                  <\/jats:p>","DOI":"10.1002\/aenm.71684","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T04:37:18Z","timestamp":1791434238000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Janus Ag Nanoskin\u2010Armored Polyimide Bilayer Separator Enables Efficient Li\u2010Nucleation Regulation for Dendrite\u2010Free Lithium Metal Battery"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5462-7525","authenticated-orcid":false,"given":"Pengpeng","family":"Li","sequence":"first","affiliation":[{"name":"Hebei Key Laboratory of Flexible Functional Materials College of Materials Science and Engineering Hebei University of Science and Technology  Shijiazhuang 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