The quantitative analysis of bioactive phenolic compounds was carried out for the first time in above-ground plant parts of Geranium dalmaticum (Beck) Rech. f. and G. macrorrhizum L. (Geraniaceae) from Croatia by means of UV-Vis spectrophotometric methods and HPLC analysis. Both species had similar contents of polyphenolic substances expressed as mg of standard equivalent /g of dried herbal sample: total polyphenols (217.60 ± 1.08 and 215.53 ± 1.10 mg/g), tannins (155.83 ± 0.60 and 157.73 ± 0.61 mg/g), total flavonoids (5.10 ± 0.10 and 5.53 ± 0.10 mg/g), and total phenolic acids (13.27 ± 1.34 and 15.33 ± 0.45 mg/g), respectively for G. dalmaticum and G. macrorrhizum. Only the content of phenolic acids was somewhat higher in G. macrorrhizum but it was not statistically significant (p > 0.05). HPLC analysis showed that, among seven tested phenolic compounds, only quercetin was quantified in G. dalmaticum (0.23 % of dry weight), and rutin in G. macrorrhizum (1.12 % of dry weight). The obtained results represent a useful basis for further research of phytochemicals and biological activities of G. dalmaticum and G. macrorrhizum extracts.