Management of Hg-contaminated sites poses particular challenges because methylmercury (MeHg), a potent bioaccumulative neurotoxin, is formed in the environment, and concentrations are not generally predictable based solely on total Hg (THg) concentrations. In this review, we examine the state of knowledge regarding the chemical, biological, and physical controls on MeHg production and identify those most critical for contaminated site assessment and management. We provide a list of parameters to assess Hg-contaminated soils and sediments with regard to their potential to be a source of MeHg to biota and therefore a risk to humans and ecological receptors. Because some measurable geochemical parameters (e.g., DOC) can have opposing effects on Hg methylation, we recommend focusing first on factors that describe the potential for Hg bioaccumulation: site characteristics, Hg and MeHg concentrations, Hg availability, and microbial activity, where practical. At some sites, more detailed assessment of biogeochemistry may be required to develop a conceptual site model for remedial decision making. Integr Environ Assess Manag 2017;13:249-263. C 2016 SETAC