Allium ursinumL. is a wild relative of garlic, and it is abundant in many antioxidant compounds. Sulfur compounds, primarily cysteine sulfoxides (CSOs), are converted through several reactions into various volatile molecules, which are considered the principal flavor compounds of Alliums. In addition to secondary metabolites, wild garlic is abundant in primary compounds, such as amino acids, which serve not only as building blocks for the health-promoting sulfur compounds but also as antioxidants. The aim of this study was to investigate the link between individual amino acid contents, the total phenolic content, and the profile of volatile compounds as well as their influence on the antioxidant capacity of both the leaves and bulbs of wild garlic populations in Croatia. Both univariate and multivariate methods were used to study the differences in the phytochemical compositions among the wild garlic plant organs and the link between individual compounds and antioxidant capacity. Both the plant organ and location, as well as their interaction, have a significant impact on the content of total phenolic content, amino acids, volatile organic compounds, and the antioxidant capacity of wild garlic.