In our study, Allium nigrum L. and Allium subhirsutum L. were investigated in terms of phenolic profile, acetylcholinesterase (AChE), butyrylcholinesterase (BuChE), and tyrosinase inhibitory potentials. The colorimetric analysis revealed that the highest levels of total phenol (45.6, 15.8 mg GAE/g extract, respectively) and total flavonoid contents (8.2, 5.7 mg QE/g extract, respectively) were found in the bulbs of both plants. About 30 compounds were determined by LC-ESI-MS/MS with validated method and 3-hydroxybenzoic acid (2,188.4 μg/g extract) and p-coumaric acid (1,700.8 μg/g extract) were major phenolic acids. (-)-Epigallocatechin gallate (998.3 µg/g extract) and genistein (159.3 μg/g extract) which are neuroprotective compounds were the predominant flavonoids for A. nigrum and A. subhirsutum, respectively. Enzyme inhibitory activities of samples were performed by spectrophotometrically with 96-well microplate reader. All samples showed anti-AChE, anti-BuChE, and anti-tyrosinase activities and the aerial part of A. nigrum was the most potent (IC 6.1, 3.27, 22.31 µg/ml, respectively). PRACTICAL APPLICATIONS: Many Allium species, especially those cultivated, are consumed in different countries as food in different ways. In the literature, studies on these species have generally focused on organosulfur compounds of the species. In our present study, phenolic compounds having a wide range of biological activities were determined in different parts of the two Allium species consumed as food. We also investigated in vitro cholinesterases and tyrosinase inhibition activities of these species. A correlation was observed between phenolic compounds and enzyme inhibition activities. These results were further explored and confirmed by principal component analysis (PCA). PCA revealed that samples were discriminated from each other according to phenolic compounds and enzyme inhibitory potencies. Conclusively, this study determines that the chemical profiles and biological activities of A. nigrum and A. subhirsutum.