Surface water reservoirs provide us with reliable water supply, hydropower generation, flood control and recreation services. Yet reservoirs also cause flow fragmentation in rivers and lead to flooding of upstream areas, thereby displacing existing land-use activities and ecosystems. Anticipated population growth and development coupled with climate change in many regions of the globe suggests a critical need to assess the potential for future reservoir capacity to help balance rising water demands with long-term water availability. Here, we assess the potential of large-scale reservoirs to provide reliable surface water yields while also considering environmental flows within 235 of the world's largest river basins. Maps of existing cropland and habitat conservation zones are integrated with spatially-explicit population and urbanization projections from the Shared Socioeconomic Pathways to identify regions unsuitable for increasing water supply by exploiting new reservoir storage. Results show that even when maximizing the global reservoir storage to its potential limit (∼4.3-4.8 times the current capacity), firm yields would only increase by about 50% over current levels. However, there exist large disparities across different basins. The majority of river basins in North America are found to gain relatively little firm yield by increasing storage capacity, whereas basins in Southeast Asia display greater potential for expansion as well as proportional gains in firm yield under multiple uncertainties. Parts of Europe, the United States and South America show relatively low reliability of maintaining current firm yields under future climate change, whereas most of Asia and higher latitude regions display comparatively high reliability. Findings from this study highlight the importance of incorporating different factors, including human development, land-use activities, and climate change, over a time span of multiple decades and across a range of different scenarios when quantifying available surface water yields and the potential for reservoir expansion.