An integrated water sustainability assessment is conducive to realizing the optimal allocation and efficient water utilization, and alleviating the water crisis. Existing research mainly appraises water quantity and water quality as unidimensional or in combination, without considering the water benefit, and few studies have assessed the regional water sustainability based on an integrated evaluation multidimensionally. Therefore, this paper innovatively introduces water benefit to construct a three-dimensional quantity-quality-benefit model (QQBM) to evaluate water sustainability in line with the water footprint (WF) theory and water resources balance sheet (WRBS). The impact of the coupled coordination relationship among water quantity, water quality, and water benefit on the water sustainability evaluation is further analyzed by introducing the coupled coordination degree model (CCDM). This paper takes the Yangtze River Economic Belt (YREB) as an example and makes a spatio-temporal analysis of the water sustainability in its 11 provincial capitals during 2010-2021 from a single dimension and a three-dimensional perspective, respectively. The results found that: (1) From a single dimension, the water sustainability in the 11 provincial capitals in the YREB during 2010-2021 is at a medium level, with better water benefit sustainability, moderate water quantity sustainability, and horrendous water quality sustainability. Among them, the water sustainability is the best in Guiyang and Hangzhou, while the worst in Shanghai. (2) From a three-dimensional perspective, the water sustainability in the 11 provincial capitals from 2010 to 2021 is horrific. Among them, the water sustainability is the best in Kunming, Changsha, Nanjing and Shanghai, while the worst in Wuhan and Hefei. (3) The degree of coupling coordination between water quantity, water quality and water benefit significantly influence the water sustainability in the 11 provincial capitals of the YREB. The three-dimensional assessment model QQBM constructed in this study is more comprehensive and objective than the single perspective assessment. The findings in this paper can help other regions to conduct similar water sustainability assessments and inform policy recommendations.