Brassicaceae is one of the most popular family of vegetables consumed worldwide. Owing to their wide range of phenolic compounds, the attention of researchers has shifted towards their pharmacological exploitation. This study investigates into the antioxidant properties of three solvent extracts (acetone, methanol, and aqueous) of C. draba and D. sophia using six assays including DPPH, ABTS, CUPRAC, FRAP, phosphomolybdenum, and β-carotene/linoleic acid inhibition. Spectrophotometric and liquid chromatography-electrospray ionization-tandem mass spectrometry (LC-ESI-MS/MS) techniques were used to determine the total and individual phytocompounds, respectively. Results showed that among the C. draba extracts, the methanolic one displayed the highest antioxidant activities in CUPRAC, FRAP, and phosphomolybdenum assays while the aqueous extract exerted the strongest DPPH and ABTS scavenging, and β-carotene inhibition. As for D. sophia extracts, the acetone extract displayed the highest activity in CUPRAC and phosphomolybdenum assays; the methanol extract was the most effective DPPH scavenger while the aqueous extract showed the highest ABTS scavenging and ferric reducing power, and β-carotene inhibitory effect. Total phenolic content was highest in the acetone extract of C. draba, while the methanolic extract of D. sophia showed the highest total flavonoid content. The most abundant compounds in C. draba extract were verbascoside and chlorogenic acid, while hesperidin and hyperoside were most abundant in the extract of D. sophia. The present findings revealed that both species had potent antioxidant properties and could be utilized as new natural antioxidants for therapeutic purposes.