| Summary: | Variation in plant species and extraction solvents play a crucial role in the recovery of their bioactive compounds and antifungal efficacy. Thus, in this study, a comparative investigation was carried out using extraction solvents: 70% acetone and 95% ethanol to obtain crude aqueous extracts from <i>Helichrysum odoratissimum</i> and <i>H. patulum</i>. Crude aqueous extracts were screened using gas chromatography–mass spectrometry (GC–MS), to gain insight into their chemical composition. Phytochemical properties (total polyphenols (TP) and radical scavenging capacity via 2,2-diphenyl-1-picrylhydrazyl (DPPH)), and antifungal activity against <i>Botrytis cinerea</i> of the crude extracts were evaluated. Fungicide (Rovral<sup>®</sup> WP) and extraction solvents were used as controls. Variation in <i>Helichrysum</i> spp. and extraction solvent had influence on the chemical composition, phytochemicals, and antifungal activities. Metabolites such as γ-terpinene (≈0.1%), α-amorphene (≈0.6%) α-gurjunene (≈1.4%), β-selinene (2.2–3.2%), γ-gurjunene (≈3.3%), and methyl cinnamate (≈20%) were detected only in extracts of <i>H. patulum</i>. Crude extract of <i>H. odoratissimum</i> using 70% acetone had the highest TP (19.3 ± 0.76 g GA 100 g<sup>−1</sup>), and DPPH capacity (13,251.5 ± 700.55 µmol Trolox g<sup>−1</sup>) compared to <i>H. patulum</i> (<i>p</i> ≤ 0.05). Ethanolic extracts of <i>H. patulum</i> showed highest antifungal efficacy (≈65%) against <i>B. cinerea</i> (<i>p</i> ≤ 0.05) compared to other crude extracts. This study showed that <i>Helichrysum</i> spp. differ in their potential as a source for bioactive compounds and antifungal treatments/formulations.
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