During the last two decades, interest in cellulosic nanomaterials has greatly increased. Among these nanocelluloses, cellulose nanocrystals (CNC) exhibit outstanding properties. Indeed, besides their high crystallinity, cellulose nanocrystals are interesting in terms of morphology with high aspect ratio (length 100–1000 nm, width 2–15 nm), high specific area, and high mechanical properties. Moreover, they can be used as rheological modifier, emulsifier, or for barrier properties, and their surface chemistry opens the door to numerous feasible chemical modifications, leading to a large panel of applications in medical, electronic, composites, or packaging, for example. Traditionally, their extraction is performed via monitored sulfuric acid hydrolysis, leading to well-dispersed aqueous CNC suspensions; these last bearing negative charges (half-sulfate ester groups) at their surface. More recently, natural chemicals called deep eutectic solvents (DESs) have been used for the production of CNC in a way of green chemistry, and characterization of recovered CNC is encouraging.