Liquid crystals (LC) have been found to have many unique characteristics during the last few decades. The liquid crystal phase is ubiquitous in the biological world, as well as in cellulose and its derivatives. Cellulose nanocrystals (CNC), which can obtain the chiral LC phase in aqueous suspension, have been attracting much attention. The unique size and properties of CNC, such as their light weight, special optical properties, non-toxicity, and biocompatibility, etc., have made them widely applicable in diverse fields. This brief literature review introduces the relationship between the LC phase and CNC. Advantages of CNC as a liquid crystal forming material and the preparation of CNC are discussed. The left-handed cholesteric phase structure and the corresponding unique optical properties of CNC-based LC are described in detail. The CNC-based LC aqueous suspension and three stages of forming LC phase are also described. Then, the main reasons accounting for the brittleness and non-uniformity of pristine CNC-based LC are summarized, as well as ways to overcome these problems. Finally, some optical applications of CNC-based LC films in anti-counterfeiting, colorimetric sensors, and composite devices are considered.