Several efforts have been made by researchers to predict the sensory profile of coffee by instrumental measurement results. The aim of the work reported here was to determine the applicability of instrumental methods on coffee samples to replace the sensory analysis. For this purpose, we evaluated the most important sensory attributes of coffee capsule samples by sensory evaluation, electronic tongue and chemical analysis (SPME–GC–MS). The trained sensory panel was able to distinguish the samples based on global odor (p = 0.01), and bitter (p < 0.01), winey (p = 0.01), fruity (p < 0.01) taste attributes. The electronic tongue distinguished the pure origin and the blended coffee samples. The aroma analysis did not find significant differences among the various coffee samples; primarily, the components formed during roasting were measured. Promising models were developed by the instrumental measurement results to predict definite sensory attributes, e.g., in case of global odor intensity (R = 0.99, RMSECV = 1.56), acidity (R = 0.96, RMSECV = 0.94).