Cellulose nanocrystals (CNCs) are an environmentally friendly natural material, consisting of rod‐like crystalline nanoparticles, called whiskers, or nanocrystalline cellulose. The derivation of different natural sources, aligned to their biocompatibility, biodegradability, and versatility, make them a class of fascinating materials with widespread industrial use. In addition, the cellulose species possess intriguing physicochemical and mechanical properties. This paper provides an overview of recent progress in the area of cellulosic nanocomposites, along with details of their structure and liquid crystalline behavior as nematic and cholesteric lyotropic materials. Guidance is subsequently provided for the physicochemical analysis of these materials, including X‐ray diffraction, transmission electron microscopy, optical evaluation, thermogravimetric analysis, and differential scanning calorimetry. Additionally, the functional chemical and physical properties of CNCs are correlated to the resulting nanotoxicity in in vitro and in vivo assays. This review points to relevant concerns, such as sources for the synthesis of CNCs, the nanomaterial size, and the surface chemistry, that must be overcome in order to attain safe use of CNC‐based nanomaterials. The challenging perspectives on the ongoing research are presented in order to explore the technological and industrial perspectives on the use of CNC for the generation of cost‐effective advanced nanomaterials based on cellulosic fibers.

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