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This chapter considers the synthesis, properties, and applications of polymer composites with a high filler content (≥30 wt%) of cellulose nanoparticles, that is, cellulose nanofibres (CNFs) and nanocrystals (CNCs). Approaches to the synthesis of high content filler polymer nanocomposites are suggested to facilitate the maximum reinforcement of cellulose nanoparticles. The synthesis involves several structures such as one-dimensional (1-D) fibre, two-dimensional (2-D) film, and three-dimensional (3-D) structure. The comparison between nanocellulose-based fibres with natural plant-based fibres is outlined. Recent studies such as crustacean mimetic cellulose film and 3-D printing of nanocellulose are emphasized. The physical and chemical limitations for the synthesis of high cellulose content composites as well as their existing and future applications are considered. The advantages of using high filler content polymer composites are discussed. A summary of progress is offered, and the future outlook is highlighted.

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