The chemical composition of essential oils and hydrosols of immortelle (Helichrysum italicum) stems with leaves obtained by hydrodistillation was identified using gas chromatography coupled with mass spectrometry (GC-MS). One-year-old and two-year-old plants of the same immortelle population, and plants from three Croatian populations, all grown in Slovenia, were included in the study. The main compounds of essential oils of one-year-old and two-year-old plants were α-pinene, α-eudesmol, and rosifoliol. Among essential oils of the Croatian populations, three dominant components were found: α-pinene, geranyl acetate, and 2-phenylethyl tiglate. Both the essential oils and hydrosols of one-year-old plants were more diverse in their compositions than two-year-old plants. The predominant compounds of hydrosols of one- and two-year-old plants were pentan-3-one, 3-octanone, 2,2-dimethylnon-5-en-3-one, and α-terpineol, and in the Croatian populations α-terpineol, 2,6-octadien-1-ol, 2,2-dimethylnon-5-en-3-one, and α-terpineol.