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Despite the important role vegetation plays in the global water cycle, the exact controls of vegetation water use, especially the role of soil biogeochemistry, remain elusive. In this study, we reveal a new mechanism of soil biogeochemical control of large-scale vegetation water use. Nitrate and sulfate deposition from fossil fuel burning have caused substantial soil acidification, leading to the leaching of soil base cations. Of these, calcium has a unique role in plant cells by regulating stomatal aperture, thus affecting vegetation water use. We hypothesized that the leaching of the soil calcium supply, induced by acid deposition, would increase large-scale vegetation water use. We present evidence from a long-term whole watershed acidification experiment demonstrating that the alteration of the soil calcium supply by acid deposition can significantly intensify vegetation water use (~10% increase in evapotranspiration) and deplete available soil water. These results are critical to understanding future water availability, biogeochemical cycles, and surface energy flux and to help reduce uncertainties in terrestrial biosphere models.