Natal plum fruit (Carissa macrocarpa) is indigenous to South Africa and a rich source of cyanidin derivatives. Indigenous fruits play a major role in food diversification and sustaining food security in the Southern African region. Agro-processing of indigenous are practiced adopted by the rural African communities in order to reduce the postharvest wastage of fruit commodities. In the current study, Natal plum was added to mango pulp at different ratios (mango and Natal plum (5:1, 3:1, 2:1)) to develop a healthy-functional snack (fruit leather). The effects of added Natal plum on the availability of antioxidant constituents and in vitro antioxidant properties of a mango-based fruit leather were evaluated by comparing with mango fruit leather. Fruit leather containing mango and Natal plum (2:1) retained the highest content of cyanidin-3-O-glucoside chloride, cyanidin- 3-O-β-sambubioside, epicatechin, apigenin, kaempferol, luteolin, quercetin-3-O-rhamnosyl glucoside, catechin, quinic, and chlorogenic acids, and in vitro antioxidant activity. Proximate analysis showed that 100 g of fruit leather (2:1) contained 63.51 g carbohydrate, 40.85 g total sugar, 0.36 g fat, and 269.88 cal. Therefore, enrichment of mango fruit leather with Natal plum (2:1) increases its phytochemical content and dietary phytochemical intake, especially for school children and adolescents.