Although a vast number of Aloe species are known, only the Aloe vera and Aloe arborescens species are currently used by cosmetic and pharmaceutical industries. Therefore, the current study aims to complete the existent literature data with new information on the phytochemical composition of some lesser-known Aloe species, with the main focus on carotenoids and fatty acids. Among the analyzed species, Aloe aculeata and Aloe ferox had the highest content in carotenoids, the major pigments being lutein and β-carotene (according to HPLC analysis). The fatty acid profile of each Aloe species was analysed by GC-MS. Linolenic and linoleic acids were the major polyunsaturated fatty acids found in higher percent in Aloe ferox, Aloe spectabilis and Aloe marlothii. Instead, Aloe aculeata proved to have a distinct fatty acid profile, rich in monounsaturated fatty acids. Species such as Aloe arborescens and Aloe marlothii proved to have the highest antioxidant potential according to data of DPPH, ORAC, HPS assays, even if the richest one in vitamin C was found to be Aloe spectabilis. Though the scientific research is mainly focused on the common species Aloe barbadensis, current data suggests that other Aloe species could receive more attention from industry part, being great sources of bioactive compounds.