Phlegrean mandarin fruits are already known for health-promoting properties due to the high concentration of phytochemicals in peel, pulp, and seed. Biotic and abiotic factors, including light, may modulate their biosynthesis, metabolism, and accumulation. In this context, light-emitting diodes (LED) have recently been applied to control nutritional traits, ripening process, senescence, fruit shelf-life, and pathogenic microbial spoilage of fruits. This study investigated the effect of the seven-day exposure of Phlegrean mandarin fruits to two LED regimes, white (W) and red–blue (RB), to test the possibility that the storage under specific light wavelengths may be used as green preservation technology that enhances fruit phytochemical properties. To pursue this aim, the antioxidant activity and polyphenolic profile of the pulp and peel of mandarins under W and RB light regimes were evaluated and compared with Control fruits not exposed to LED treatment. Our results indicated that storage under W and RB treatments modulates the antioxidant content in pulp and peel differently. Compared to W, the RB regime increases the ascorbic acid, flavonoid, anthocyanin, and carotenoid concentrations, while the polyphenol profile analysis reveals that the number of important phytochemicals, i.e., quercetin rutinoside, chlorogenic acid, sinensetin, and rutin, are higher under W. The overall data demonstrated that postharvest LED irradiation is a valid tool for modifying fruit phytochemical properties, which also boosts specific bioactive compounds