Cellulose nanocrystals (CNC) with high aspect ratio of 50 have been readily prepared from the inexpensive fruit shell of Camellia oleifera Abel (SCOA) for the first time. In this study, SOCA was consecutively subjected to sulfite pulping and acid hydrolysis to remove non-cellulosic components，release CNC and prepare highly transparent film. The derived CNC possesses a needle-shaped structure that in average diameter and length of 8 ± 2 nm and 400 ± 100 nm, respectively. The crystallinity index of CNC increased to 72% and the initial decomposition temperature raised to 230 °C. The obtained CNC was formed to nanopaper by vacuum filtration showing high visible light transmittance over 80 % and high strength. Thus SOCA derived CNC is of great practical potential to apply in the field of food packaging.