Cellulose nanocrystals (CNCs) extracted from the waste shell of Camellia oleifera Abel (C. oleifera) are gaining attention as valuable materials. In this study, CNCs were extracted from the agricultural waste shell of C. oleifera through phosphoric acid and sulfuric acid hydrolysis, respectively. Firstly, we optimized the alkaline treatment process for cellulose isolation by using response surface methodology. Furthermore, the properties of CNCs were investigated by neutralizing them with NaOH and NH₃·H₂O, and by dialysis in water. In addition, the characterization methods including FTIR, TGA, AFM and TEM were used to analysis the properties of the synthesized CNCs. Finally, CNCs were studied for their application in essential oil-based Pickering emulsions. CNCs obtained from sulfuric acid showed the smallest particle size and good dispersibility. Moreover, the release profiles of essential oils in the emulsions were followed by Peppa's kinetic release model. The antibacterial activity of the emulsions against E. coli and S. aureus showed that CNCs-stabilized emulsions enhanced the antibacterial activity of essential oils. Therefore, neutralization treatments may enhance the properties of CNCs, and CNCs stabilized Pickering emulsions can enhance antibacterial activity of essential oil. This study provides insight into the potential application of CNCs derived from C. oleifera waste shells.