Adverse health outcomes, including death from cardiovascular disease (CVD), arising from chronic exposure to inorganic arsenic (iAs) are well documented. Consumption of rice is a major iAs exposure route for over 3 billion people, however, there is still a lack of epidemiological evidence demonstrating the association between iAs exposure from rice intake and CVD risks. We explored this potential association through an ecological study using data at local authority level across England and Wales. Local authority level daily per capita iAs exposure from rice (E-iAsing,rice) was estimated using ethnicity as a proxy for class of rice consumption. A series of linear and non-linear models were applied to estimate the association between E-iAsing,rice and CVD age-standardized mortality rate (ASMR), using Akaike’s Information Criterion as the principle model selection criterion. When adjusted for significant confounders, notably smoking prevalence, education level, employment rate, overweight percentage, PM2.5, female percentage and medical and care establishments, the preferred non-linear model indicated that CVD risks increased with iAs exposure from rice at exposures above 0.3 µg/person/day. Also, the best-fitted linear model indicated that CVD ASMR in the highest quartile of iAs exposure (0.375-2.71 µg/person/day) was 1.06 (1.02, 1.11; p-trend < 0.001) times higher than that in the lowest quartile (< 0.265 µg/person/day). Notwithstanding the well-known limitations of ecological studies, this study further suggests exposure to iAs including from rice intake as a potentially important confounder for studies of the factors controlling CVD risks.