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Herein, we report a versatile and robust coating (pBDT\u2010TA), self\u2010assembled from tannic acid (TA) and a self\u2010polymerizing aromatic dithiol (i.e., benzene\u20101,4\u2010dithiol, BDT), that can be engineered on diverse substrates with a precisely tuned thickness (5\u201340\u2005nm) by varying the concentration of BDT used. The pBDT\u2010TA coating is stabilized by covalent (disulfide) bonds and supramolecular (\u03c0\u2010\u03c0) interactions, endowing the coating with high stability in various harsh aqueous environments across ionic strength, pH, temperature (e.g., 100\u2005mM NaCl, HCl (pH\u20051) or NaOH (pH\u200513), and water at 100\u2009\u00b0C), as well as surfactant solution (e.g., 100\u2005mM Triton X\u2010100) and biological buffer (e.g., Dulbecco's phosphate\u2010buffered saline), as validated by experiments and simulations. Moreover, the reported pBDT\u2010TA coating enables secondary reactions on the coating for engineering hybrid adlayers (e.g., ZIF\u20108 shells) via phenolic\u2010mediated adhesion, and the facile integration of aromatic fluorescent dyes (e.g., rhodamine B) via \u03c0 interactions without requiring elaborate synthetic processes.<\/jats:p>","DOI":"10.1002\/anie.202106316","type":"journal-article","created":{"date-parts":[[2021,7,13]],"date-time":"2021-07-13T22:52:37Z","timestamp":1626216757000},"page":"20225-20230","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":37,"title":["Robust and Versatile Coatings Engineered via Simultaneous Covalent and Noncovalent Interactions"],"prefix":"10.1002","volume":"60","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5203-4737","authenticated-orcid":false,"given":"Jiajing","family":"Zhou","sequence":"first","affiliation":[{"name":"ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, and the Department of Chemical Engineering The University of Melbourne  Parkville Victoria 3010 Australia"},{"name":"Department of NanoEngineering University of California San Diego  9500 Gilman Dr. La Jolla CA 92093 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Matthew","family":"Penna","sequence":"additional","affiliation":[{"name":"School of Engineering RMIT University  Melbourne Victoria 3001 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9372-3424","authenticated-orcid":false,"given":"Zhixing","family":"Lin","sequence":"additional","affiliation":[{"name":"ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, and the Department of Chemical Engineering The University of Melbourne  Parkville Victoria 3010 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4547-3368","authenticated-orcid":false,"given":"Yiyuan","family":"Han","sequence":"additional","affiliation":[{"name":"ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, and the Department of Chemical Engineering The University of Melbourne  Parkville Victoria 3010 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0026-3428","authenticated-orcid":false,"given":"Ren\u00e9 P. M.","family":"Lafleur","sequence":"additional","affiliation":[{"name":"ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, and the Department of Chemical Engineering The University of Melbourne  Parkville Victoria 3010 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yijiao","family":"Qu","sequence":"additional","affiliation":[{"name":"ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, and the Department of Chemical Engineering The University of Melbourne  Parkville Victoria 3010 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8618-4127","authenticated-orcid":false,"given":"Joseph J.","family":"Richardson","sequence":"additional","affiliation":[{"name":"ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, and the Department of Chemical Engineering The University of Melbourne  Parkville Victoria 3010 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