CALCIUM is the fifth most abundant element in trees, and is an essential component for wood formation and the maintenance of cell walls. Depletion of Ca from the rooting zone can result in acidification of soil1 and surface water2 and possibly growth decline and dieback of red spruce3,4. During the past six decades, concentrations of root-available Ca (exchangeable and acid-ex tract able forms) in forest-floor soils have decreased in the northeastern United States5,6. Both net forest growth and acid deposition have been put forth as mechanisms that can account for this Ca depletion5,6. Here, however, we present data collected in red spruce forests in the northeastern United States that are inconsistent with either of these mechanisms. We propose that aluminium, mobilized in the mineral soil by acid deposition, is transported into the forest floor in a reactive form that reduces storage of Ca, and thus its availability for root uptake. This results in potential stress to trees and, by increasing the demand for Ca, also decreases neutralization of drainage waters, thereby leading to acidification of lakes and streams.