Water sustainability in megacities is a growing challenge with far reaching effects. Addressing sustainability requires an integrated, multidisciplinary approach able to capture interactions among hydrology, population growth, and socioeconomic factors and to reflect changes due to climate variability and land use. We developed a new systems modeling framework to quantify the influence of changes in land use, crop growth, and urbanization on groundwater storage for Beijing, China. This framework was then used to understand and quantify causes of observed decreases in groundwater storage from 1993-2006, revealing that the expansion of Beijing’s urban areas at the expense of croplands has enhanced recharge while reducing water lost to evapotranspiration, partially ameliorating groundwater declines. The results demonstrate the efficacy of such a systems approach to quantify the impacts of changes in climate and land use on water sustainability for megacities, while providing a quantitative framework to improve mitigation and adaptation strategies that can help address future water challenges.