To alleviate the water shortage in northern China, the Chinese government launched the world's largest water diversion project, the South-to-North Water Diversion Project (SNWDP), which delivers water from water-sufficient southern China to water-deficient northern China. However, an up-to-date study has not been conducted to determine whether the project is a favorable option to augment the water supply from an environmental perspective. The life cycle assessment (LCA) methodology integrated with a freshwater withdrawal category (FWI) was adopted to compare water supply alternatives in the water-receiving areas of the SNWDP, i.e., water diversion, wastewater reclamation and seawater desalination. Beijing, Tianjin, Jinan and Qingdao were studied as representative cities because they are the primary water-receiving areas of the SNWDP. The results revealed that the operation phase played the dominant role in all but one of the life cycle impact categories considered and contributed to more than 70% of their scores. For Beijing and Tianjin, receiving water through the SNWDP is the most sustainable option to augment the water supply. The result can be drawn in all of the water-receiving areas of the middle route of the SNWDP. For Jinan and Qingdao, the most sustainable option is the wastewater reclamation system. The seawater desalination system obtains the highest score of the standard impact indicators in all of the study areas, whereas it is the most favorable water supply option when considering the freshwater withdrawal impact. Although the most sustainable water supply alternative was recommended through an LCA analysis, multi-water resources should be integrated into the region's water supply from the perspective of water sustainability. The results of this study provide a useful recommendation on the management of water resources for China.