Eight non-centrifugal cane brown sugars were compositionally differentiated by their sugar, amino acid, mineral, phenolic, and volatile aroma components. Their taste and aroma profiles were generated using two electronic sensing techniques, namely, a potentiometric electronic tongue (e-tongue) and a mass spectrometry (MS)-based electronic nose (e-nose). The nutritional and phenolic contents varied in brown sugars and influenced relative taste values for sweetness, umami, astringency, and bitterness. Various composition–taste correlations, including both contributive and negative associations, were discovered, whereas minerals and phenolics had a positive effect on astringency and bitterness. Brown sugars were also composed of different formations of volatile aroma components, predominantly acetaldehyde, ethanol, acetic acid, butanoic acid, 2,5-dimethyl pyrazine, and 2,6-dimethyl pyrazine. Hyphenated MS-based e-nose sensing differentiated brown sugars in more detail and generated important discriminant chemical markers for those aroma compounds in the multivariate PCA statistical model, viz., m/z 42 and 43 (acetaldehyde), 46 (ethanol), 55 and 73 (butanoic acid), 60 (acetic acid), and 94, 108, and 122 (pyrazines).