The present study aimed to evaluate the antioxidant and enzyme inhibition properties of aerial part of Verbascum cheiranthifolium Boiss. V. myriocarpum Boiss. & Heldr. and V. pyroliforme (Boiss. & Heldr.) Kuntze as well as their chemical profiles. Results showed that MeOH and hydromethanol recovered the highest total polyphenolic content with highest content obtained from V. cheiranthifolium (27.61and 27.69 mg GAE/g respectively) and V. myriocarpum (24.24 and 25.34 GAE/g respectively). The estimated content of verbascoside was quite higher in V. cheiranthifolium (987.05–6780.07 mg/100 g) and V. myriocarpum (1506.47–6433.73 mg/100 g) than V. pyroliforme (49.54–121.97 mg/100 g). All extracts of V. cheiranthifolium (274.17–713.79 mg/100 g) and polar ones of V. myriocarpum (185.67–304.51 mg/100 g) accumulated higher chlorogenic acid content than V. pyroliforme extracts (36.33–112.56 mg/100 g). The latter species was dominated by luteolin-7-O-glucoside and apigenin-7-O-glucoside with highest content recorded from the hydromethanolic extract (639.70 and 196.14 mg/100 g respectively). Extracts of V. cheiranthifolium (46.15–48.74 mg TE/g) and V. myriocarpum (46.05–48.50 mg TE/g) exerted significantly higher scavenging activity than those from V. pyroliforme (12.77–34.64 mg TE/g). Highest significant anti-acetylcholinesterase activity was obtained by MeOH extract of V. pyroliforme (2.65 mg GALAE/g) and V. myriocarpum (2.57 mg GALAE/g). In conclusion, extracts from the three investigated Verbascum spp. can be a potential source of bioactive metabolites with interesting antioxidant and enzyme inhibition properties.