Sample measurement of mercury (Hg) contents is a common method for health risk assessment of Hg through vegetable consumption in China. In the present work, we undertook the first modelling study which produced consistent health-risk maps for the whole eastern China. Regional maps of Probable Daily Intake (PDI) of Total mercury (THg) and Methylmercury (MeHg) over the studied area were produced, which were important for the researchers and policy-makers to evaluate the risk and to propose mitigation measures if necessary. The model predictions of air-borne Hg(0) concentrations agreed well with the observations and simulated Hg distribution over China as reported elsewhere. Our calculated PDIs of THg in vegetables were also comparable to those reported in the literature. There was 19% of the studied area with PDIs > 0.08 μg kg−1 bw d−1 [half of the reference dose (RfD)]. The PDI for THg (MeHg) varied from 0.034 (0.007) to 0.162 (0.035) μg kg−1 bw d−1 with an average of 0.058 (0.013) μg kg−1 bw d−1. The highest calculated PDIs of THg over China was equal to the RfD, while the calculated PDIs of MeHg were well below the RfD of 0.1 μg kg−1 bw d−1. The health risk was of concern through consumption of THg in leafy vegetables, rice/wheat and fish in Liaoning Provinces, Hunan, Zhejiang and Guizhou Provinces, with the associated PDIs exceeding the RfD. Despite this, the heath risk of MeHg exposure for the general population in southern China from the same foodstuff consumption was not a concern. The contribution of consumption through leafy vegetation should be considered when THg and MeHg exposures to the population are evaluated. The results improve our understanding in managing public health risk in China especially in large cities with high population, and thus have important contribution to enhance sustainable urbanization as one of the principle goals under the framework of the Nature-Based Solution (NBS).