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Nanocellulose, the most abundant crystalline polysaccharide nanomaterial on Earth, has been widely used for the reinforcement of polymeric materials owing to its high elastic modulus, low density, high aspect ratio, biocompatibility, and biodegradability. In this Perspective, we offer a brief overview of recent progress in the controllable arrangement of nanocellulose in polymeric matrices, including highly oriented structure, helical structure, and gradient structure. We then discuss the current nanotechnologies that enable the arrangeme