Snow and ice-core samples from a number of sites in Antarctica and Greenland have been analyzed for the major anions Cl−, NO3 −, and SO4 2- by ion chromatography. Reproducibility on adjacent core or pit samples is ±10% at the 95% confidence level. Chloride is of marine origin except following some major volcanic eruptions. Chloride concentrations decrease exponentially with increasing site elevation with a scale height of about 1.5 km. For sites of comparable elevation, Antarctic Cl− concentrations are only slightly higher than in Greenland. Sulfate concentrations, corrected for the marine aerosol contribution, show an inverse dependence on snow accumulation rate. For sites of comparable accumulation rate, Greenland concentrations exceed those in Antarctica by a factor of 2 to 3. Nitrate concentrations also decrease with increasing accumulation rate and for comparable sites Greenland NO3 − concentrations are a factor of 2 higher than in Antarctica. There is no evidence of solar modulation or supernova perturbation of Greenland NO3 − concentrations. The Byrd deep core is shown to have distinct seasonal variations in Cl− and SO4 2- that may be used for dating. In addition, the Byrd core contains volcanic signals similar to those found in Greenland. Recent Greenland snow contains about 4 times as much SO4 2- and 2 to 3 times as much NO3 − as is found in older ice due to modern fossil fuel combustion.