In this study, the effects of sequential fermentation ofLachancea thermotolerans/S. cerevisiaeon the production of Plavac Mali wines were investigated in comparison with the commonly used inoculation of the commercialSaccharomyces cerevisiaestrain and spontaneous fermentation. A total of 113 aroma compounds and 35 polyphenolic compounds were analyzed. Sequential inoculation resulted in a decrease in alcohol content and pH (up to 0.3%v/vand 0.12 units, respectively) and an increase in total acidity (0.6 g/L, expressed as tartaric acid). The wines produced by spontaneous fermentation exhibited the greatest diversity of volatile compounds and the highest concentration of C13 norisoprenoids, lactones, and other compounds. These wines exhibited maximum hydroxycinnamic acids, prodelphinidin monomer units, epigallocatechin, B1, B3, and B4 dimers, and total flavan-3-ols. Sequential inoculation decreased the content of the aromas and polyphenols in the wines. The practical significance of this procedure lies in the selective effect on aroma compounds, the decrease in green aromas, undetectable volatile phenols, and the decrease in bitter and astringent compounds such as gallic acid, flavan-3-ol monomers (catechin and epicatechin), and dimers (B1, B2, B3, and B4). This work demonstrates the potential of sequential and spontaneous fermentation to improve the aromatic characteristics and overall quality of Plavac Mali wines.