We report the largest market basket survey of arsenic (As) in U.S. rice to date. Our findings show differences in transitional-metal levels between polished and unpolished rice and geographical variation in As and selenium (Se) between rice processed in California and the South Central U.S. The mean and median As grain levels for the South Central U.S. were 0.30 and 0.27 μg As g-1, respectively, for 107 samples. Levels for California were 41% lower than the South Central U.S., with a mean of 0.17 μg As g-1 and a median of 0.16 μg As g-1 for 27 samples. The mean and median Se grain levels for the South Central U.S. were 0.19 μg Se g-1. Californian rice levels were lower, averaging only 0.08 and 0.06 μg Se g-1 for mean and median values, respectively. The difference between the two regions was found to be significant for As and Se (General Linear Model (GLM):  As p < 0.001; Se p < 0.001). No statistically significant differences were observed in As or Se levels between polished and unpolished rice (GLM:  As p = 0.213; Se p = 0.113). No significant differences in grain levels of manganese (Mn), cobalt (Co), copper (Cu), or zinc (Zn) were observed between California and the South Central U.S. Modeling arsenic intake for the U.S. population based on this survey shows that for certain groups (namely Hispanics, Asians, sufferers of Celiac disease, and infants) dietary exposure to inorganic As from elevated levels in rice potentially exceeds the maximum intake of As from drinking water (based on consumption of 1 L of 0.01 mg L-1 In. As) and Californian state exposure limits. Further studies on the transformation of As in soil, grain As bioavailability in the human gastrointestinal tract, and grain elemental speciation trends are critical.