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Nanocomposites consisting of cellulose nanofibrils (CNFs) and nano-aluminum nitride (AlN) were prepared using a simple vacuum-assisted filtration process. Bleached sugarcane bagasse pulp was treated with potassium hydroxide and sodium chlorite, and was subsequently ultra-finely ground and homogenized to obtain CNFs. Film nanocomposites were prepared by mixing CNFs with various AlN amounts (0–20 wt.%). X-ray diffraction revealed that the crystal form of CNF-AlN nanocomposites was different to those of pure CNFs and AlN. The mechanical performance and thermal stability of the CNF-AlN nanocomposites were evaluated through mechanical tests and thermogravimetric analysis, respectively. The results showed that the CNF-AlN nanocomposites exhibited excellent mechanical and thermal stability, and represented a green renewable substrate material. This type of nanocomposite could present great potential for replacing traditional polymer substrates, and could provide creative opportunities for designing and fabricating high-performance portable electronics in the near future. [ABSTRACT FROM AUTHOR]