Humans are exposed to toxic methylmercury mainly by consuming marine fish. The Minamata Convention aims at reducing anthropogenic mercury releases to protect human and ecosystem health, employing monitoring programs to meet its objectives. Tunas are suspected to be sentinels of mercury exposure in the ocean, though not evidenced yet. Here, we conducted a literature review of mercury concentrations in tropical tunas (bigeye, yellowfin, and skipjack) and albacore, the four most exploited tunas worldwide. Strong spatial patterns of tuna mercury concentrations were shown, mainly explained by fish size, and methylmercury bioavailability in marine food web, suggesting that tunas reflect spatial trends of mercury exposure in their ecosystem. The few mercury long-term trends in tunas were contrasted and sometimes disconnected to estimated regional changes in atmospheric emissions and deposition, highlighting potential confounding effects of legacy mercury, and complex reactions governing the fate of mercury in the ocean. Inter-species differences of tuna mercury concentrations associated with their distinct ecology suggest that tropical tunas and albacore could be used complementarily to assess the vertical and horizontal variability of methylmercury in the ocean. Overall, this review elevates tunas as relevant bioindicators for the Minamata Convention, and calls for large-scale and continuous mercury measurements within the international community. We provide guidelines for tuna sample collection, preparation, analyses and data standardization with recommended transdisciplinary approaches to explore tuna mercury content in parallel with observation abiotic data, and biogeochemical model outputs. Such global and transdisciplinary biomonitoring is essential to explore the complex mechanisms of the marine methylmercury cycle.