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Studies on African medicinal plants have been limited to some geographically areas, and even though more than 5400 medicinal plants are recognized and documented, other valuable medicinal plant species have not been studied. Ethnopharmacological studies are important for documenting traditional knowledge associated with the medical use of biodiversity. This study aims to document the use of medicinal plants from the Province of Cuanza Norte (Angola). The field work was conducted from December 2018 to January 2019 and the ethnobotanical data were collected using semi-structured interviews. Informants were selected in accordance with their residence and community recognition as healers. Recorded plants are listed along with their popular name, traditional use, part used, and method of preparation. A total of 131 species of medicinal plants were cited. Mukumbi (Lannea welwitschii), Santa Maria (Chenopodium ambrosioides) and Ditumbata (Boerhavia difusa) were the most cited species. Out of the total plant parts, leaves were the most frequently material used. Regarding the mode of preparation for the medicinal materials, the major form of preparation is maceration, followed by infusion and decoction. The main categories of use were infectious and parasitic diseases (e.g., Malaria); undefined pains and illness; diseases of the digestive system; and endocrine, nutritional, and metabolic diseases (e.g., Diabetes). This study revealed the importance of preserving the ethnobotanical knowledge in order to protect the biodiversity and to discover new therapeutic molecules. A comparison of the results with other studies showed that some of the traditional indications are supported by data from scientific literature.