Due to high water content and perishability, the raspberry fruit is sensitive to postharvest fungal contamination and postharvest losses. In this study, chitosan was used as an edible coating to increase the storage of raspberries, and nanotechnology was used to increase chitosan efficiency. The fruit was treated with an emulsion containing nanoparticles of chitosan (ECNPC) at 0, 2.5, and 5 g L−1, and stored for 9 d. Decay extension rate, fruit phytochemical contents, including total phenolics, flavonoids, and anthocyanin content, phenylalanine ammonia-lyase (PAL), and guaiacol-peroxidase enzymes and antioxidant activity, and other qualitative properties were evaluated during and at the end of storage. After 9 d of storage, the highest amounts of phenolics compounds, PAL enzyme activity, and antioxidant activity were observed in fruit treated with ECNPC at 5 g L−1. The highest levels of total phenol, PAL enzyme activity, and antioxidant activity were 57.53 g L−1, 118.88 μmol/min trans-cinnamic acid, and 85.16%, respectively. ECNPC can be considered as an effective, safe, and environmentally friendly method for enhancing fruit phytochemical contents, postharvest life, and health-promoting capacity.