Mercury (Hg) contamination is an issue of a growing environmental and public health concern. Atmospheric chemistry transport models for Hg are a critical tool for understanding the sources, processes, and fate of Hg. Uncertainties in multiple aspects of atmospheric Hg models, however, limit their application for policy evaluation and for monitoring global trends in atmospheric Hg concentrations. This review aims to identify uncertainties in atmospheric Hg modeling that are relevant in the context of policy and for informing decision-making. We focus on specific requirements of the Minamata Convention on Mercury, a global treaty signed in 2013 to protect human health and the environment from Hg, to demonstrate how existing uncertainties in atmospheric Hg modeling can influence our ability to evaluate source-receptor relationships. Modeling studies of source attribution suggest that major uncertainties in atmospheric Hg modeling arise from anthropogenic emissions, biogeochemical cycling, and atmospheric chemistry. Uncertainties in these aspects of modeling are expected to increase under the Convention, with regulation of anthropogenic emissions, changes in atmospheric conditions, and legacy and natural Hg source contribution to the global biogeochemical cycle. These uncertainties can interact with one another and with the current Hg species measurement capability and pose challenges to effectively monitoring trends in atmospheric Hg. Developing additional means to attribute simulated atmospheric Hg trends and improve source-receptor relationships in atmospheric Hg models would improve our ability to evaluate the Convention's effectiveness.