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Ethnopharmacological context Cape herbal medicine as a distinct and unique healing system is conceptualized for the first time, together with a first compilation of the authentic materia medica of the system.Materials and methods The early literature on Khoikhoi (Hottentot), San (Bushman) and Cape Dutch medicinal plants and medical practices is reviewed, with a focus on the Cape Floristic Region (from Namaqualand to the Eastern Cape). To avoid recent additions and modern cultural influences in the results, the date of publication of the last volume of Marloth's Flora of South Africa (1932) was chosen as a cut-off date.Results The recorded Cape materia medica (up to 1932) is briefly summarized, giving the scientific names, vernacular names (in Afrikaans or Khoi-San/Nama) and main uses. It comprises about 170 items and includes mainly indigenous and endemic plant species, some exotic (garden) plants, and a few other items (fungi, seaweeds, lichens, hyraceum and natural potassium nitrate). Most of the plants (and hyraceum) are still widely used today, especially in rural areas.Conclusions The combination of unique cultural practices and a diverse, highly endemic flora has led to the development of a distinct herbal healing system, here called Cape herbal medicine, but hitherto rather vaguely and inaccurately referred to as Khoi-San medicine, Cape Dutch medicine or boererate (farm remedies). The data allows for a more informed consideration of indigenous knowledge and intellectual property rights associated with particular plants (e.g. Hoodia and Pelargonium). It also offers opportunities for linking modern ethnobotanical field studies with historical data.