Leguminosae is an economically important family that contains a large number of medicinal plants, many of which are widely used in African traditional medicine. Angola holds a great socio-cultural diversity and is one of the richest floristic regions of the world, with over 900 native Leguminosae species. This study is the first to assess the medicinal uses of the legumes in Angola and provides new data to promote the conservation and the sustainable use of these unique resources. We document the ethnobotanical knowledge on Angola by reviewing the most important herbarium collections and literature, complemented by recent field surveys. Our results revealed that 127 native legume species have medicinal uses and 65% of them have other important uses by local populations. The species with most medicinal applications are and . The rich flora found in Angola suggests an enormous potential for discovery of new drugs with therapeutic value. However, the overexploitation and the indiscriminate collection of legumes for multiple uses such as forage, food, timber and medical uses, increases the threats upon the native vegetation. Efforts to assess the conservation status of these species are urgently needed, and future actions should promote the sustainable use of medicinal plants in Angola together with the implementation of conservation strategies.