In this study, phytochemical and pharmacological screening of the aerial part and roots extracts from Doronicum orientale Hoffm. (Asteraceae) was carried out. Plant extracts were obtained using solvents of different polarity (hexane, ethyl acetate, ethanol, ethanol/water, water) for selection the most optimal solvent for the extraction of active compounds. For instance, the extracts yielded total phenolic and flavonoid contents in the range of 12.13–45.67 mg GAE/g and 0.75–12.44 mg QE/g, respectively, while the total antioxidant capacity of the extracts determined by the phosphomolybdenum assay ranged from 0.88–2.53 mmol TE/g. HPLC/MS/MS analysis revealed 5-caffeoylquinic acid (2.52–337.05 μg/g) and 3,5-dicaffeoylquinic acid (3.12–299.36 μg/g) to be the major components present in the investigated extracts. Antioxidant activity in terms of radical scavenging ability of the extracts ranged from 0.82–45.56 mg TE/g in DPPH assay and from 5.07–104.58 mg TE/g in ABTS assay. The tested extracts were found to inhibit acetylcholinesterase (aerial part: 0.50–2.33 mg GALAE/g; roots: 0.40–2.43 mg GALAE/g), while with the exception of the water extracts, the other extracts showed butyrylcholinesterase inhibition (aerial part: 2.46–5.02 mg GALAE/g; root: 2.93–4.17 mg GALAE/g). Overall, this study presented an interesting scope of this species in phytomedicine with preliminary data demonstrating some of the tested extracts to possess high bioactive contents, antioxidant potential and enzyme inhibitory activity. Thus, additional investigations are necessary to confirm their safety in herbal drug applications.