The aim of this study was to assess the health risk attributable to the consumption of mercury-contaminated fish for the urban and non-urban populations living in the Roraima state, Amazon, Brazil. Seventy-five fish specimens distributed across twenty different species, comprising four trophic levels (i.e., herbivore, omnivore, detritivore, and carnivore), were collected at four locations in the Branco River Basin. The fish samples were sent to the Toxicology Laboratory at Evandro Chagas Institute to determine the total-Hg levels by using the cold vapor atomic system (CVAAS). The total-Hg levels ranged from 0 to 3.159 µg/g. The average concentration in non-carnivorous species (n = 32) was 0.116 µg/g, and among carnivorous fish (n = 43), it was 0.869 µg/g. The weighted average of contamination levels for all samples was 0.545 µg/g. The health risk assessment was conducted according to the methodology proposed by the World Health Organization and different scenarios of human exposure were considered, based on three levels of fish consumption (low: 50 g/day; moderate: 100 g/day and high: 200 g/day). Women of childbearing age ingest 5 to 21 times more mercury than the dose considered safe by the U.S. EPA and intake a dose from 2 to 9 times higher than the safe dose proposed by FAO/WHO. Children under 5 years of age ingest from 18 to 75 times the dose proposed by the U.S. EPA and from 8 to 32 more mercury than the limit proposed by FAO/WHO. In summary, regardless of the level of fish consumption, type of residency (urban or non-urban), and the subset of the population analyzed, anyone who consumes fish from the locations sampled is at high risk attributable to mercury ingestion, with the only exception of adult men, who consume an average of 50 g of fish per day.