Mango (Mangifera indica Linn.) is a famous climacteric fruit containing abundant flavor and nutrients in the tropics, but it is prone to decay without suitable postharvest preservation measures. In this study, the chitosan (CH)-cinnamon essential oil (CEO) Pickering emulsion (CH-PE) coating was prepared, with cellulose nanocrystals as the emulsifier, and applied to harvested mangoes at the green stage of maturity. It was compared with a pure CH coating and a CH-CEO emulsion (CH-E) coating, prepared with the emulsifier Tween 80. Results showed that the CH-PE coating had a lower water solubility and water vapor permeability than the other coatings, which was mainly due to electrostatic interactions, and had a better sustained-release performance for CEO than the CH-E coating. During mango storage, the CH-PE coating effectively improved the appearance of mangoes at 25 °C for 12 d by reducing yellowing and dark spots, and delayed water loss. Hardness was maintained and membrane lipid peroxidation was reduced by regulating the activities of pectin methyl esterase, polygalacturonase, and peroxidase. In addition, the nutrient quality was improved by the CH-PE coating, with higher contents of total soluble solid, titratable acid, and ascorbic acid. Therefore, the CH-PE coating is promising to comprehensively maintain the postharvest quality of mangoes, due to its enhanced physical and sustained-release properties.