Croton heliotropiifolius Kunth and Croton argyrophyllus Kunth are endemic plant species from northeastern Brazil widely used in folk medicine and scarcely studied. In this context, the essential oils (EO's) and methanolic extracts (leaves and stalk) of both species were chemically characterized, and their antioxidant and antimicrobial activities were assessed. The chemical characterization of the EO's identified sixty components,being the major ones in C. argyrophyllus bicyclogermacrene (14.0%), β-pinene (8.9%) and spathulenol (8.7%), and in C. heliotropiifolius limonene (16.9%), α-pinene (13.3%) and caryophyllene (12.1%). Essential oils and methanolic extracts from leaves of C. argyrophyllus possess greater antioxidant potential, which could be related to the high levels of total phenols and flavonols. The antimicrobial activity of C. argyrophyllus essential oil proven to be more efficient than chloramphenicol (30 μg mL −1 ), with a minimum inhibitory concentration (MIC) of 25 μL mL −1 against Bacillus subtilis, Staphylococcus aureus, Escherichia coli and Pseudomonas aeruginosa and 10 μL mL −1 against B. cereus. Leaf extracts presented high activity against yeasts (MIC = 50 mg mL −1 ) being C. heliotropiifolius effective against Candida albicans and C. parapsilosis, while C. argyrophyllus was effective against C. glabrata. Overall results showed that these plant species are potential sources of phytochemicals with interest in the fields of both pharmacology (e.g., antimicrobial) and human health (e.g., antioxidant). Furthermore, in the socio-economic aspect, these results can improve and disseminate the cultivation of these species, inducing improvements in the rural populations.