The antioxidant activity, general toxicity and cytotoxicity of the methanol extracts of Centaurea urvillei subs. armata and C. mucronifera have been assessed, respectively, by the DPPH assay, the brine shrimp lethality and the MTT cytotoxicity assays. The reversed-phase HPLC analysis of the methanol extracts afforded two bioactive dibenzylbutyrolactone-type lignans, matairesinoside (1) and arctiin (2). The structures of these lignans were elucidated by comprehensive spectroscopic analyses as well as by the direct comparison of experimental data with respective literature data.