Chromatic variation was examined for its association with flour composition and quality. Carob samples from variable altitudes and genetic backgrounds were milled and assessed for colorimetric parameter L* (lightness) and analyzed for phenols, tannins, antioxidant capacity, soluble carbohydrates (HPLC-RID), organic acids and protein (IC-CD), and volatile organic compounds (VOCs; HS-SPME/GC-MS). Higher altitudes and grafted genotypes yielded lighter-colored flours of higher antioxidant potential, phenols, tannins, sucrose, and malic acid concentrations. VOCs were mainly acids, esters, aldehydes, ketones, and alcohols. Acids were the most abundant and correlated negatively with L*, though correlation for many individual acids was non-significant, including 2-methyl-propanoic acid, widely considered the carob signature aroma (cheesy acidic buttery). The compositional and quality indexing potential of L* is more robust for grafted than non-grafted material, owing putatively to a narrower genetic basis. Antioxidant capacity and concentrations of phenolics, tannins and sucrose correlated positively with L*, indicating increased levels in carob flours sourced from grafted trees at higher altitudes. These flours also have a lower content of reducing sugars, the implication of which in the darkening of carob flour warrants further investigation. Overall, L* constitutes a reliable index for ranking carob flours for key compositional attributes and may be further reinforced by multiple-year data.