Water resources carrying capacity is an important indicator for evaluating the sustainable use of regional water resources. To evaluate regional water resources carrying capacity quantitatively, a multi-level evaluation system was established based on water resources-society-economy-ecological environment system. Considering the shortcomings of the traditional set pair analysis (SPA) model, the grey cluster set pair analysis model was constructed by introducing the center triangle whitening weight function, and its index weights were determined by game theory. Anhui Province as an example was given to demonstrate the accuracy and effectiveness of the evaluation model and the evaluation results were basically in accord with the actual situation. The results showed that water resources carrying capacity in Anhui province in 2008-2013 was evaluated as Class Ⅲ, and ClassⅡin 2014-2017, which indicates that the water resources carrying capacity in this area had been improved effectively. Based on ArcGIS visualization function, the regional difference analysis of water resources carrying capacity of 16 cities in Anhui Province was demonstrated. It shows that the north-south difference in Anhui Province was obvious, and the south water resources carrying capacity was better than that of the north, which is related to the uneven distribution of water resources, different social development patterns and regional ecological environment differences. For the sustainable development of social economy in Anhui Province, a suitable and applicable scheme of sustainable utilization of water resources should be formulated based on the characteristics of the regional development and the current situation of its ecological environment.