Background: Cellulose is a ubiquitous, renewable and environmentally friendly biopolymer, which has high promise to fulfil the rising demand for sustainable and biocompatible materials. Particularly, the recent progress in the synthesis of highly crystalline cellulose-based nanoscale biomaterials, namely cellulose nanocrystals (CNCs), draws significant attention from many research communities, ranging from bioresource engineering, to materials science and engineering, to biological and biomedical engineering to bionanotechnology. The feasibility of harnessing CNCs' unique biophysicochemical properties has inspired their basic and applied research, offering much promise for new biomaterials with diverse advanced functionalities. Purpose: This review focuses on vital issues and topics on the recent advances in CNC-based biomaterials with potential, in particular, for bionanotechnology and biological and biomedical engineering. The challenges and limitations of CNC technology are discussed as well as potential strategies to overcome them, providing an essential source of information in the exploration of possible and futuristic applications of the CNC-based functional "green" nanomaterials. Conclusion: CNCs offer exciting possibilities for advanced "green" nanomaterials, driving innovative research and development in a wide range of fields, including biological and biomedical engineering.