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In the present work, four different types of cellulose nanofibres (CNFs), two types of clay minerals used individually (sepiolite) or combined (sepiolite + kaolinite), and the influence of pH, were explored in the production of composite films. Neat CNFs, only mechanically treated or prepared by enzymatic pre-treatment, gave films with good mechanical and barrier properties, but the addition of minerals led to a dramatic loss of these properties. Contrarily, the use of thin and functionalized fibrils (TEMPO-oxidised or cationized CNFs) gave composite films with good mechanical, thermal and barrier properties. Superior oxygen barrier properties (oxygen transmission rate (OTR)\u2009&lt;\u20090.4\u00a0cm<jats:sup>3<\/jats:sup>\u00a0m<jats:sup>\u22122<\/jats:sup>\u00a0day<jats:sup>\u22121<\/jats:sup>) were obtained using TEMPO-oxidised CNF and 20% sepiolite, and, in general, for all the composite films containing the TEMPO CNF\u00a0(OTR\u2009\u2264\u20091.8\u00a0cm<jats:sup>3<\/jats:sup>\u00a0m<jats:sup>\u22122<\/jats:sup>\u00a0day<jats:sup>\u22121<\/jats:sup>). The cationic CNF-based composites also showed a very good oxygen barrier (OTR\u2009\u2264\u20098.2\u00a0cm<jats:sup>3<\/jats:sup>\u00a0m<jats:sup>\u22122<\/jats:sup>\u00a0day<jats:sup>\u22121<\/jats:sup>). The high oxygen barrier could be explained by the compactness of the films and better entanglement of the more fibrillated nanocelluloses with the mineral particles. A decrease in the pH of the suspensions led to a decrease in the film preparation time, without a major negative impact on the composite film\u2019s properties.<\/jats:p>","DOI":"10.1007\/s10570-023-05495-z","type":"journal-article","created":{"date-parts":[[2023,9,20]],"date-time":"2023-09-20T04:02:30Z","timestamp":1695182550000},"page":"10157-10174","update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":24,"title":["Design of cellulose nanofibre-based composites with high barrier properties"],"prefix":"10.1007","volume":"30","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4447-5107","authenticated-orcid":false,"given":"Lu\u00eds","family":"Alves","sequence":"first","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7324-1070","authenticated-orcid":false,"given":"Ana","family":"Ramos","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4717-6305","authenticated-orcid":false,"given":"Eduardo","family":"Ferraz","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4503-6811","authenticated-orcid":false,"given":"Paulo J. 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