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Supplementary data to this article can be found online at https://doi.org/10.1016/j.foodres.2020.108983, Calcium supplements have increasingly been used at pre-harvest stages for improving fruit firmness, aiming at mitigating environmental stress. However, as recent studies demonstrated that calcium modifies the polyphenolic profile of grape berries, we hypothesize in this study that it also affects wine volatile profile. In a two-year study, grapevines cv. Vinhão were sprayed with 2% CaCl2 throughout the fruiting season, and musts were prepared at a laboratory scale. Musts from calcium-treated fruits contained higher calcium levels and less anthocyanins. Increased calcium content did not affect the course of fermentation induced with a S. cerevisiae starter inoculum, but impacted the course of spontaneous fermentations carried out by endogenous berry microflora. Several compounds associated to varietal and fermentative aromas were largely influenced by the calcium treatment. For instance, volatile phenols decreased, together with -damascenone, benzaldehyde and -nonalactone, while several acetates and alcohols increased. Principal component analysis showed that the volatile profile of control wines produced by spontaneous fermentation substantially differed between replicates, but calcium treatment lowered replicate variability. Volatile profiles were also influenced by the vintage and fermentation type. The shift in wine volatile profile upon calcium treatment may be relevant from an oenological perspective., This work was supported by the Portuguese Foundation for Science and Technology (FCT) in the framework of the strategic funding [UID/BIA/04050/2019, UID/AGR/04033/2019] and the projects [PTDC/AGR-PRO/7028/2014, PTDCBIA-FBT/28165/2017, PTDC/BIA-FBT/30341/2017, and SFRH/BPD/107905/2015 to V.M.]., info:eu-repo/semantics/publishedVersion