The largest source of global mercury (Hg) anthropogenic inputs to the environment is derived from artisanal and small-scale gold mining (ASGM) activities in developing countries. While our understanding of global Hg emissions from ASGM is growing, there is limited empirical documentation about the levels of total mercury (THg) and methylmercury (MeHg) contamination near ASGM sites. We measured THg and MeHg concentrations in soil (n = 119), sediment (n = 22), and water (n = 25) from four active ASGM villages and one non-ASGM reference village in Senegal, West Africa. Nearly all samples had THg and MeHg concentrations that exceeded the reference village concentrations and USEPA regulatory standards. The highest median THg concentrations were found in huts where mercury-gold amalgams were burned (7.5 μg/g), while the highest median MeHg concentrations and percent Hg as MeHg were found in river sediments (4.2 ng/g, 0.41%). Median river water concentrations of THg and MeHg were also elevated compared to values at the reference site (22 ng THg/L, 0.037 ng MeHg/L in ASGM sites). This study provides direct evidence that Hg from ASGM is entering both the terrestrial and aquatic ecosystems where it is converted in soils, sediment, and water to the neurotoxic and bioavailable form of MeHg.