China’s South–North Water Transfer Project (SNWTP) has the potential to transfer as much as 44.8 km³ year^-1 of water from the Yangtze River basin to the Yellow River basin. However, the SNWTP has not been assessed from a sustainability perspective. Thus, in this study we evaluated the SNWTP’s economic, social, and environmental impacts by reviewing the English literature published in journals that are part of the Web of Science database. We then synthesized this literature using a Triple Bottom Line framework of sustainability assessment. Our study has led to three main findings: (1) whether the SNWTP is economically beneficial depends largely on model assumptions, meaning that economic gains at the regional and national level are uncertain; (2) the SNWTP requires the resettlement of hundreds of thousands of people and challenges existing water management institutions, suggesting possible social concerns beyond the short term; and (3) evidently large environmental costs in water-providing areas and uncertain environmental benefits in water-receiving areas together point to an uncertain environmental future for the geographic regions involved. Thus, the overall sustainability of SNWTP is seriously questionable. Although much work has been done studying individual aspects of SNWTP’s sustainability, few studies have utilized the multi-scale, transdisciplinary approaches that such a project demands. To minimize environmental risks, ensure social equity, and sustain economic benefits, we suggest that the project be continuously monitored in all three dimensions, and that integrated sustainability assessments and policy improvements be carried out periodically.