Besides specific, incidental radiation exposure, which has been associated with increased thyroid cancer risk, the effects of exposure to background radiation from uranium, a naturally occurring, radioactive, and ubiquitous element, on the thyroid gland has not been widely studied. We therefore investigated the association between uranium exposure and thyroid health in the US. Using the National Health and Nutrition Examination Survey (NHANES), we assessed the association between urinary uranium levels and thyroid-related antibodies, including thyroglobulin antibodies (TgAb) and anti-thyroid peroxidase (anti-TPO), in the general population. Secondly, we performed an ecological study of age-adjusted thyroid cancer incidence rates per state and sources of uranium exposure. We included 3125 eligible participants from the NHANES and found a significant association between increased TgAb and increased urinary uranium levels when analyzed as quartiles (p = 0.0105), while no association was found with anti-TPO. In addition, although no significant correlation was found in the ecological study, certain states had high age-adjusted thyroid cancer incidence rates and a high number of uranium activity locations and high uranium concentrations in water. The present study suggests that uranium exposure may affect thyroid health, which warrants increased sampling of soil and water in high-risk states.