In this study, mango fruit (Tainong No. 1) was treated with either 0.1 mg/L 1-methylcyclopropene (1-MCP) alone or with a combination of 0.1 mg/L 1-MCP and 0.2 mM melatonin (MT). The mango fruit was then stored for 10 days at 25 °C and 85–90% relative humidity. Quality characteristics and the active oxygen metabolism of postharvest mangoes were evaluated every 2 days. Compared to untreated mango fruit, those with the treatments of 1-MCP alone or 1-MCP + MT had a better appearance and higher levels of soluble sugar, ascorbic acid, and titratable acidity. Moreover, these treatments prevented the loss of fruit firmness, successfully delayed the escalation of a* and b* values, and reduced malondialdehyde content and superoxide anion generation rate. After 10 days of storage, mango fruit treated by 1-MCP alone or 1-MCP + MT exhibited increased activities of antioxidant enzymes such as ascorbate peroxidase, catalase, superoxide dismutase, and other peroxidases; nevertheless, the two treatment protocols maintained higher mango total phenolic content only at the later stage of storage. These findings suggest that mango fruit treated with 1-MCP alone or with 1-MCP + MT improves the quality characteristics and antioxidant activities. Moreover, compared to 1-MCP treatment alone, 1-MCP + MT-treated mangoes exhibited higher quality and a stronger regulation of active metabolism during storage.