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This study presents the first report on phenolic composition and bioactivity of ethanolic extracts of three plant species that grow in the western Balkan mountains and are used in traditional folk medicine: <i>Valeriana montana</i>, <i>Salix retusa</i>, and <i>Campanula hercegovina</i>. Phenolics were extracted from different aerial plant parts using 80% ethanol to assess the possibility of sustainable use of these plants as a source of bioactive compounds without disruption to the roots (for <i>V. montana</i>) or destruction of whole habitats (for <i>S. retusa</i> and <i>C. hercegovina</i>). The ethanolic extract of <i>V. montana</i> flower contained noticeable levels of apigenin and quercetin. The branches and bark of <i>S. retusa</i> were significantly rich in catechin, while rutin was the major phenolic found in the leaf extract of <i>C. hercegovina</i>. Furthermore, the flower extract of <i>V. montana</i> revealed the best antioxidant activity, which was comparable to 4-hydroxybenzoic acid and quercetin. Considering antimicrobial activity, the leaf extracts of <i>V. montana</i> and <i>C. hercegovina</i> demonstrated potent activity against all microbes tested, while the extracts of <i>S. retusa</i> were moderately effective. The presented results emphasize the potential of these plants as novel sources of bioactive compounds.