Mercury (Hg) speciation and the activity of Hg(II)-methylating bacteria are responsible for the rate of methylmercury production and thus bioaccumulation in marine foodwebs. Factors affecting porewater partitioning (Kd) and methylation of Hg(II) were examined at 11 sites in sediment of 4 biogeochemically diverse estuaries in the Northeast U.S. In Long Island Sound, 88% of total mercury (HgT) log Kd variability was described by porewater dissolved organic carbon concentration and sediment total sulfur (S) content. Whereas across all estuaries, regression analyses showed that S alone drives about 70% of Kd variability and 50% of changes in methylation rates; and the inclusion of DOC and sulfides did not improve the prediction. Thus, we demonstrated that S is a better predictor of HgT log Kd than the sediment organic matter across multiple estuaries, and while organic matter and S are interchangeable in small-scale studies, on a larger scale, sediment S content is the simplest and most effective variable to measure.