Nanocrystalline cellulose is an abundant and inexhaustible organic material on Earth. It can be derived from many lignocellulosic plants and also from agricultural residues. They endowed exceptional physicochemical properties, which have promoted their intensive exploration in biomedical application, especially for tissue engineering scaffolds. Nanocrystalline cellulose has been acknowledged due to its low toxicity and low ecotoxicological risks towards living cells. To explore this field, this review provides an overview of nanocrystalline cellulose in designing materials of bone scaffolds. An introduction to nanocrystalline cellulose and its isolation method of acid hydrolysis are discussed following by the application of nanocrystalline cellulose in bone tissue engineering scaffolds. This review also provides comprehensive knowledge and highlights the contribution of nanocrystalline cellulose in terms of mechanical properties, biocompatibility and biodegradability of bone tissue engineering scaffolds. Lastly, the challenges for future scaffold development using nanocrystalline cellulose are also included.