Global pollution has exacerbated accumulation of toxicants like methylmercury (MeHg) in seafood. Human exposure to MeHg has been associated with long-term neurodevelopmental delays and impaired cardiovascular health, while many micronutrients in seafood are beneficial to health. The largest MeHg exposure source for many general populations originates from marine fish that are harvested from the global ocean and sold in the commercial seafood market. Here, we use high-resolution catch data for global fisheries and an empirically constrained spatial model for seafood MeHg to examine the spatial origins and magnitudes of MeHg extracted from the ocean. Results suggest that tropical and subtropical fisheries account for >70% of the MeHg extracted from the ocean because they are the major fishing grounds for large pelagic fishes and the natural biogeochemistry in this region facilitates seawater MeHg production. Compounding this issue, micronutrients (selenium and omega-3 fatty acids) are lowest in seafood harvested from warm, low-latitude regions and may be further depleted by future ocean warming. Our results imply that extensive harvests of large pelagic species by industrial fisheries, particularly in the tropics, drive global public health concerns related to MeHg exposure. We estimate that 84 to 99% of subsistence fishing entities globally likely exceed MeHg exposure thresholds based on typical rates of subsistence fish consumption. Results highlight the need for both stringent controls on global pollution and better accounting for human nutrition in fishing choices.