The Harlem coal is postulated to have been deposited in raised-bog settings. It was initially deposited as low-sulfur peat, but groundwater of a later origin altered portions of it to high-sulfur coal. The total sulfur content of 172 samples from 31 locations on a moisture-and ash-free basis have a quadrimodal distribution with two major modes at 0.75% S and 2.0% S. Multiple sampling and analyses at specific mine sites indicate that the addition of sulfur of a later origin occurred either laterally adjacent to sandstone channels or vertically adjacent to faults. Significant sulfur addition also occurred above clay partings at these sites. The original low-sulfur nature is preserved where the coal bed is isolated from descending groundwater by a thick impervious layer. Trace-element analyses show high concentrations of mobile elements such as Na and Mn in the high-sulfur coals.