Harvest time is major factor of affecting fruit and wine quality of grape. But quantify evaluation of wine quality according to harvest time is too difficult. We conducted this study to identify the metabolites, affecting the sensory, quality and fruit characters of grapevine cv. 'Cheongsoo' at the different harvest times, using proton spectroscopy. Our results showed that there was a clear separation of the spectrum data on the PCA plot at each harvest time. In addition, the S-plot of OPLS-DA was useful to identify the essential metabolites across the harvest times. Tartaric acid (δ4.47) was a main factor responsible for the titratable acidity and the acidity of the wine on the sensory test. In addition, both proline (δ2.37) and arginine (δ3.25) are nitrogen source during wine fermentation, and they were closely associated with the body and balance of the wine on the sensory test. The relative concentration of proline was increased across the harvest times, and it was a positive factor that is associated with changes in the body and balance of the wine. In conclusion, our results indicate that the metabolic profiling based on NMR spectroscopy, combined with a multivariate analysis, is useful in identifying metabolites that are responsible for quality of grape and wine.