Sediment from lakes on abandoned coal mines in the Midwestern U.S.A. was examined to determine the factors controlling chemical composition and the role the sediment plays in lake neutralization. Sediment concentrations of many cations, (especially heavy metals) are strongly correlated with sediment sulfide concentration, but poorly correlated with the pH of the overlying water. Leaching the sediment of one lake with 1 N ammonium acetate, 0.1 N HCl, and 6 N HCI revealed that cations were mostly bound in weak acid-leachable and strong acid-leachable forms. The weak acid-leachable form is likely to be metal sulfides and calcium carbonate. The sulfide-poor sediments of extremely acid lakes contained few weak acid-leachable cations. Raw mine-spoil contained large amounts of easily leached cations. There is little relationship between changes in sediment chemistry over time determined from cores of lake sediment and past lake pH. Rates of sulfide deposition were examined in sediment cores because sulfate reduction and deposition has been suggested as a major source of alkalinity in lakes influenced by acid precipitation. Although the rate of sulfate deposition in surface mine lakes is high, it alone seems to be insufficient to cause neutralization.