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Cuticle of mussel byssal threads, containing Fe\u2010catecholate complexes, shows remarkably high hardness, high extensibility, and self\u2010healing capability. Understanding strengthening and self\u2010healing mechanisms is essential for elucidating animal behaviors and rationally designing mussel\u2010inspired materials. Here, direct evidence of Fe<jats:sup>3+<\/jats:sup> and Fe<jats:sup>2+<\/jats:sup> gradient distribution across the cuticle thickness is demonstrated, which shows more Fe<jats:sup>2+<\/jats:sup> inside the inner cuticle, to support the hypothesis that the cuticle is a functionally graded material with high stiffness, extensibility, and self\u2010healing capacity. The mechanical tests of the mussel threads show that both strength and extensibility of the threads decrease with increasing oxygen contents, but this property degradation can be restored upon removing the oxygen. The first\u2010principles calculations explain the change in iron coordination, which plays a key role in strengthening, degradation, and self\u2010healing of the polymer networks. The oxygen absorbs on metal ions, weakening the iron\u2010catecholate bonds in the cuticle and collagen core, but this process can be reversed by sea water. These findings can have important implications in the design of next\u2010generation bioinspired robust, highly extensible materials, and catalysis.<\/jats:p>","DOI":"10.1002\/advs.201902043","type":"journal-article","created":{"date-parts":[[2019,10,24]],"date-time":"2019-10-24T13:13:46Z","timestamp":1571922826000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":64,"title":["Metal Coordination\u2010Mediated Functional Grading and Self\u2010Healing in Mussel Byssus Cuticle"],"prefix":"10.1002","volume":"6","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2195-2513","authenticated-orcid":false,"given":"Quan","family":"Xu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of Biogas Upgrading Utilization Harvard SEAS\u2010CUPB Joint Laboratory on Petroleum Science College of New Energy and Materials Science China University of Petroleum\u2010Beijing  Beijing 102249 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