Wine is an alcoholic beverage, consisting of several compounds in various ranges of concentrations. Wine quality is usually assessed by a sensory panel of trained personnel. Electronic tongues (e-tongues) and electronic noses (e-noses) have been established in recent years to assess the quality of beverages and foods. Response surface and electronic analysis tools were used to examine the quality of black tea wine. The results indicated the optimum initial sugar level (25 °Brix), yeast addition (0.5%), and fermentation temperature (25 °C) for Golden Peony black tea wine. The black tea wine produced under these conditions with 14.0% vol alcohol has as an orange-red color, full wine and tea flavor, and mild and mellow taste. The sourness of the wine was most affected by fermentation factors-yeast addition, fermentation temperature, and initial sugar level. Alcohols, aldehydes, ketones, and alkanes contributed to most of the volatile components under the influence of yeast addition and fermentation temperature. In contrast, nitrogen oxides, aromatics, and organic sulfides contributed under the influence of the initial sugar level. This study provided a facilitated strategy for obtaining the optimum black tea wine fermentation process through electronic nose and tongue-based techniques. The analysis of wines requires new technologies able to detect various different compounds simultaneously, providing worldwide information about the sample instead of information about specific compounds.