Physalis alkekengi L. (Solanaceae) is encountered in different regions of Bulgaria as a wild growing or ornamental plant. All aerial parts of the plant have been used in folk medicine for centuries due to the presence of various bioactive metabolites; the plant is included within the scope of the Medicinal Plants Act of Bulgaria. The objective of this work was to characterize the phytochemical composition of the leaves and stems of two genotypes of P. alkekengi collected from natural habitats in Southern and Northern Bulgaria (PA-SB and PA-NB), with the view of revealing their use potential in feed, cosmetics and other areas. The results from the study revealed significant differences in the levels of the phytochemical components (ash, cellulose, protein, amino acids, macro and micro minerals), both on a plant part and genotype basis. The leaves of the two genotypes were further processed by extraction with n-hexane, for the identification of leaf volatiles. The GC-MS analysis identified 28 components (97.99%) in the leaf extract of PA-SB, and 32 components (97.50%) in that of PA-NB. The volatile profile of PA-SB leaves was dominated by diterpenes (49.96%) and oxygenated sesquiterpenes (35.61%), while that of PA-NB – by oxygenated aliphatics (40.01%) and diterpenes (35.19%). To the best of our knowledge, the study provides the first data about the content of macro and micro nutrients and volatiles in the leaves and stems of P. alkekengi from Bulgaria, in a direct comparison of genotypes from two distinct populations, which could be of further practical interest.