A field survey of mercury pollution in environmental media and human hair samples obtained from residents living in the area surrounding the Chatian mercury mine (CMM) of southwestern China was conducted to evaluate the health risks of mercury to local residents. The results showed that mine waste, and tailings in particular, contained high levels of mercury and that the maximum mercury concentration was 88.50 μg g−1. Elevated mercury levels were also found in local surface water, paddy soil, and paddy grain, which may cause severe health problems. The mercury concentration of hair samples from the inhabitants of the CMM exceeded 1.0 μg g−1, which is the limit recommended by the US EPA. Mercury concentrations in paddy soil were positively correlated with mercury concentrations in paddy roots, stalks, and paddy grains, which suggested that paddy soil was the major source of mercury in paddy plant tissue. The average daily dose (ADD) of mercury for local adults and preschool children via oral exposure reached 0.241 and 0.624 μg kg−1 body weight per day, respectively, which is approaching or exceeds the provisional tolerable daily intake. Among the three oral exposure routes, the greatest contributor to the ADD of mercury was the ingestion of rice grain. Open-stacked mine tailings have resulted in heavy mercury contamination in the surrounding soil, and the depth of appreciable soil mercury concentrations exceeded 100 cm.