γ-Aminobutyric acid (GABA) plays important roles in plant development, including the maintenance of fruit quality when applied as postharvest treatment. However, little information is available about the effects of preharvest GABA treatments. Thus, GABA (10, 50 and 100 mM) was applied as foliar spray at key points of fruit development in three sweet cherry cultivars and over two years. The results show that quality parameters, such as total soluble solid content, titratable acidity and firmness were higher in the fruit from GABA-treated trees than in the controls, either at harvest or during four weeks of cold storage. In addition, the total phenolic and total and individual anthocyanin concentrations were also enhanced by GABA treatments and the fruit color was improved. The activities of the antioxidant enzymes catalase, ascorbate peroxidase and peroxidase were also enhanced by the GABA treatments. The most effective concentration was 50 mM, which led to extending the storage period of sweet cherries with high quality traits to up to four weeks, while for the controls this was two weeks. Thus, GABA treatment had a clear effect on delaying the postharvest ripening and senescence processes in sweet cherries, with an additional effect on enhancing the content of bioactive compounds, such as phenolics and anthocyanins, with antioxidant properties and health benefits.