Aloe species are among the most significant plants with several applications. Many of the species, however, are underexplored, owing to their scarcity and limited geographical distribution. A. adigratana Reynolds, which is common in Ethiopia, is one of the little-studied and endangered Aloe species. This preliminary study focuses on the phytochemical screening, proximate analysis, essential oil content, and antifungal activities of A. adigratana leaf peels. Antifungal activities were also tested on the gels of the plant for comparison. Standard procedures were used for phytochemical and proximate composition studies. Essential oil analysis was performed using a gas chromatography-mass spectrometry instrument. Using the well-diffusion method, investigations on antifungal activity were performed on three clinically isolated specimens of dandruff-causing fungus; namely, Malassezia furfur, Malassezia restricta, and Malassezia globosa. The leaf peels of A. adigratana contained alkaloids, flavonoids, tannins, and terpenes. The mean moisture, ash, and crude fat levels were 85.69, 92.20, and 8.00%, respectively, whereas the mean total protein and mean total carbohydrate values were 2.59 and 3.04%. Gas chromatography-mass spectrometry investigation confirmed the presence of fifteen essential oils. The most prevalent essential oil component was discovered to be phytol (33.78%), followed by decane (11.29%). In a dose-dependent way, the leaf latex and gel extracts prevented the growth of three dandruff-causing Malassezia fungal species (M. furfur, M. restricta, and M. globosa). Both the latex and gel demonstrated the maximum activity on M. globosa, the most prevalent fungus in the research area, with minimum inhibitory concentrations of 0.24 and 0.48 mg/mL and minimum fungicidal concentrations of 0.48 and 0.97 mg/mL, respectively. In general, the proximate and essential oil compositions of A. adigratana leaves were comparable to those of other Aloe species widely used in the food, cosmetic, and pharmaceutical industries, implying that A. adigratana could be a potential future plant for such industries.