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Here, we report a waterborne interfacial reinforcement and functionalization strategy to construct multifunctional natural rubber latex (NRL)\u2010based bioelastomers. Ammonium persulfate (APS)\u2010assisted treatment promotes interfacial coupling between NRL chains and cellulose nanofibers (CNFs), establishing nanofiber\u2010mediated load\u2010transfer and energy\u2010dissipation pathways. ZnO nanoparticles introduce inorganic physical junctions that regulate interfacial stress transfer while providing UV shielding and antibacterial activity. The optimized NRL\u2010g\u2010CNF\/ZnO composite exhibits a tensile strength of 9.68\u00a0MPa, toughness of 15.30\u00a0MJ\u00b7m\n                    <jats:sup>\u22123<\/jats:sup>\n                    , and efficient room\u2010temperature self\u2010healing, with tensile strength and toughness recovery of 96.9% and 92.8% after 48\u00a0h, respectively. The composite also shows pronounced crack tolerance, including a fracture energy of 32.5\u00a0kJ\u00b7m\n                    <jats:sup>\u22122<\/jats:sup>\n                    and stable deformation of notched samples, together with improved short\u2010term mechanical retention under the specified UV\u2010aging conditions, antibacterial activity, a measurable soil\u2010burial response, and preliminary cytocompatibility. This simple casting\u2010based strategy provides a potentially scalable route to multifunctional bioelastomers with potential for selected packaging applications, protective coatings, antibacterial\/UV\u2010shielding films, and non\u2010implantable flexible materials.\n                  <\/jats:p>","DOI":"10.1002\/adma.74584","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T14:11:22Z","timestamp":1786371082000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Waterborne Interfacial\u2010Reinforcement Strategy for Sustainable Natural Rubber Latex Bioelastomers With Self\u2010Healing, Crack Tolerance, and Multifunctional Durability"],"prefix":"10.1002","volume":"38","author":[{"given":"Dongna","family":"Li","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bio\u2010based Fiber Materials Tianjin University of Science &amp; Technology  Tianjin P.R. 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