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Aloysia Paláu is an important herbal genus from the Verbenaceae family and possesses numerous remedial properties in the folk medicine of Asian, European, and, in particular, South American countries. Only a few reports have discussed some phytochemical characteristics associated with Aloysia species. Right the lack of an exhaustive report prompted us to organize this review article. Accordingly, besides the ethnobotanical knowledge of Aloysia species, their essential oil profiles, phytochemistry of the polar isolated fractions, and the relevant biological activities are discussed in detail.