The phenolic composition and in vitro antioxidant properties of solid residues from the distillation of eight populations of Salvia lavandulifolia were investigated to select the most suitable plant materials to yield natural antioxidants. The residues showed a very different phenolic content and composition, populations SL1, SL5, SL7, and SL8 showed a good total phenolic content, and comparable results in the assays of 2,2-diphenyl-1-picrylhydrazyl (DPPH) and Ferric-Reducing Antioxidant Power (FRAP), and in the inhibition of the oxidation of linoleic acid, and consequently, seemed the most promising sources of antioxidant compounds. On the other hand, SL2, SL3, and SL4 showed remarkable iron-chelating activities and could be of interest in the prevention of the oxidation process with participation of this metal through Fenton's reaction. The differences observed among residues in the phenolic composition had an apparently scarce influence on the activities investigated.