Mercury is a ubiquitous pollutant of global concern but the threat of exposure is not homogenously distributed at local, regional, or global scales. The primary route of human exposure to mercury is through consumption of aquatic foods, which are culturally and economically important in the wider Caribbean Region, especially for Small Island Developing States (SIDS). We compiled more than 1600 samples of 108 unique species of fish and aquatic invertebrates collected between 2005 and 2023 from eleven countries or territories in the wider Caribbean Region. There was wide variability in total mercury concentrations with 55% of samples below the 0.23 µg/g wet weight (ww) guideline from the U.S. FDA/EPA (2022) for 2 or 3 weekly servings and 26% exceeding the 0.46 µg/g ww guideline consistent with adverse effects on human health from continual consumption, particularly for sensitive populations. Significant relationships were found between total mercury concentrations and taxonomic family, sampling country, fish length, and trophic level. The data analyzed here support the need for further sampling with concrete geospatial data to better understand patterns and mechanisms in mercury concentrations and allow for more informed decision making on the consumption of fish and invertebrates from the wider Caribbean Region as well as supporting efforts to evaluate the effectiveness of national, regional, and international mercury policies.