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High elevation alpine ecosystems—the ‘water towers of the world’—provide water for human populations around the globe. Active geomorphic features such as glaciers and permafrost leave alpine ecosystems susceptible to changes in climate which could also lead to changing biogeochemistry and water quality. Here, we synthesize recent changes in high-elevation stream chemistry from multiple sites that demonstrate a consistent and widespread pattern of increasing sulfate and base cation concentrations or fluxes. This trend has occurred over the past 30 years and is consistent across multiple sites in the Rocky Mountains of the United States, western Canada, the European Alps, the Icelandic Shield, and the Himalayas in Asia. To better understand these recent changes and to examine the potential causes of increased sulfur and base cation concentrations in surface waters, we present a synthesis of global records as well as a high resolution 33 year record of atmospheric deposition and river export data from a long-term ecological research site in Colorado, USA. We evaluate which factors may be driving global shifts in stream chemistry including atmospheric deposition trends and broad climatic patterns. Our analysis suggests that recent changes in climate may be stimulating changes to hydrology and/or geomorphic processes, which in turn lead to accelerated weathering of bedrock. This cascade of effects has broad implications for the chemistry and quality of important surface water resources.