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Up to date, there are no reports on the effects of combined sulfur (S) and nitrogen (N) foliar application in olive orchards on volatile compounds and sensory characteristics of virgin olive oil (VOO). In this work, the effects of increasing the fertilizer S and N concentration on volatile compound composition and odor and taste attributes of monovarietal VOOs of Istarska bjelica and Leccino cultivars were investigated. The volatile compounds were analyzed by gas chromatography with flame ionization and mass spectrometric detection after isolation by solid-phase microextraction, while sensory attributes were assessed by a professional panel. In all the investigated VOO samples, aldehydes were the most represented group of compounds, with (E)-2-hexenal as the most abundant, followed by (Z)-3-hexenal and 1-penten-3-one. Significant differences in the volatile profiles and sensory attributes were observed between VOOs from different treatments, mainly attributable to the interactions between all the factors that were investigated: treatment, cultivar, and year. Although significant interactions were noted for sensory attributes as well, the score for overall quality was generally lower for Leccino VOOs and for VOOs from both cultivars that were obtained after the highest SN dose treatment. All the samples were graded by overall sensory scores that were higher than eight and were characterized by well-pronounced fruitiness and the absence of sensory defects. The results of this study showed that foliar application of S and N significantly affects the quality of VOO, confirming that such a practice can modulate the characteristic olive oil odor and taste attributes and thus possibly influence its acceptability and preference among consumers.