87Sr/86Sr evidence from a soil chronosequence in the Hawaiian Islands demonstrates that the atmosphere supplies >85% of putatively rock-derived Sr in older sites. Initially, bedrock is the dominant source for Sr and other lithophile elements such as Ca, but high rates of weathering and leaching of the substrate by 20 ka lead to a shift to atmospheric sources. The loss of weathering inputs coincides with other physio-chemical changes in the soil and results in a steep decline of base cations in the soil pool. While these patterns imply the potential for limitation of biological productivity by low base cation supply, the atmosphere provides a supply of base cations in excess of nutritional needs, even after nearly all rock-derived base cations have been leached from the soil. This raises the possibility that P limitation in terrestrial ecosystems may develop at least as much because of low rates of atmospheric deposition of P (relative to Ca, K, and other rock-derived elements) as because of its chemical interaction in soil.