Table grape berries are classified as a perishable crop that deteriorates quickly after harvest. The application of melatonin after harvest was found to be effective for retarding senescence and slowing ripening. In the current study, we tested the influence of two melatonin concentrations (50 and 100 µmol) as a postharvest application on quality, bioactive compounds, and enzyme activities of grape berries cv “Crimson” stored at 0 ± 1 °C and 90% relative humidity (RH) for 35 days. Our results indicated that melatonin application extends the shelf-life of berries by reducing weight loss and maintaining total soluble solids (TSS), titratable acidity (TA), berry adherence strength, and firmness. Melatonin treatment also reduced pectin methyl esterase (PME) and polygalactouranase (PG) enzyme activities compared to the control. Moreover, O2•− and H2O2 rates in berries were reduced by high melatonin concentration. Moreover, peroxidase (POD) and catalase (CAT) enzyme activities were increased by melatonin application. Our findings suggested using melatonin postharvest to increase shelf life and maintain quality attributes during refrigerated storage, which could be advantageous on a large scale.