Fruits of 9 Spanish pomegranate cultivars were analyzed for quality parameters, volatile composition, and sensory profile. Volatile compounds were extracted using headspace solid phase micro-extraction (HS-SPME) and analyzed by gas chromatography-mass spectrometry (GC-MS) and flame ionization detector (GC-FID). Twenty-one compounds were found in the headspace of fresh pomegranate juices, including aldehydes, monoterpenes, and alcohols. The most abundant compounds were hexanal, limonene, trans-2-hexenal, and cis-3-hexenol. Fruits from the cultivars Mollar Elche(ME) ME14, ME1, and ME2 presented the highest values of overall liking by the consumer panel; however, their total volatiles concentration were low compared to the other pomegranate cultivars and their color intensity was intermediate. Overall consumer liking of pomegranate juices was mainly associated with the presence of monoterpenes (α-terpineol); however, high aldehydes (trans-2-hexenal) concentrations were correlated with poor overall consumer liking. Fruits from sour-sweet cultivars (PTO7 and ADO4) could improve the quality of ME pomegranate juices due to their intense color, high monoterpenes concentrations, and their moderate sourness. Practical Application: The information provided in this study proves that sour-sweet pomegranate fruits can be used in the manufacturing of pomegranate juices and will improve the sensory quality and the volatile composition of this product.