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Here it is shown that Ti3C2Tx MXene flakes can be co‐assembled with recombinant silk fibroin in aqueous suspensions with silk fibroin nanolayers uniformly covering individual flakes. These bioencapsulated flakes evolve with time due to the gradual growth of silk bundles having β‐sheet secondary organization with unique nanofibrillar morphologies extending across flake edges and forming long fringes...
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