The African continent harbours many native species with nutraceutical and pharmaceutical potential. This study reviewed underutilised crops in South Africa to determine their potential as food and herbal medicinal crops. Over 5,000 species have been identified and earmarked for their medical attributes in formal and informal setups. Researchers, plant breeders and policymakers have mostly ignored the development potential of these crops. Consequently, their value chains are poorly developed. In South Africa, there is a wide range of neglected and underutilised crops, which were historically popular and used by communities; however, over the years, they have lost their status within farming systems and been relegated to the status of neglected and underutilised. Recently, driven by the need to transition to more sustainable and resilient food systems, there has been renewed interest in their potential as food and herbal medicinal crops to establish new value chains that include vulnerable groups. They are now gaining global attention, and their conservation and sustainable utilisation are now being prioritized. The review confirmed that several of these crops possess nutraceutical and pharmaceutical properties, highlighting their potential for development as food and herbal medicines. However, current production levels are too low to meet the requirements for industrial development; research and development should focus on all aspects of their value chain, from crop improvement to utilisation. A transdisciplinary approach involving a wide range of actors is needed to develop the identified neglected and underutilised crops' potential as food and herbal medicinal crops and support the development of new and inclusive value chains.