Arsenic (As) is a major environmental pollutant and a known human carcinogen that is widely distributed in the air, soil, and water. General population is mainly exposed to As through drinking water and food from the contaminated water and soil. Arsenic in drinking water is generally well controlled now. This study was performed to estimate total and inorganic As intake and to determine the major contributing source in the Korean adult diet. The study subjects were 2117 healthy adults (922 males and 1195 females) who had not been occupationally exposed to As. Total dietary intake was studied using the 24-h recall method, which included 138 specific food items. The estimates of total As and inorganic As intake were based on total and inorganic As contents in each food item consumed during the last 24 h. Daily dietary intake was estimated to be 1373.6 g. Total As intake was estimated to be 145.4 µg As/day. Total dietary As intake was correlated with consumption of fish/shellfish, seaweeds, and grains. Approximately 87% of total dietary As intake was attributed to seafood, such as 105.5 µg As/day from fish/shellfish and 20.5 µg As/day from seaweeds. Inorganic As intake was estimated to be 10.4 µg As per day. Inorganic As intake was mainly provided by grains (6.4 µg As/day), followed by seaweeds and fish/shellfish. Our results indicate that seafood and grains are the main As dietary sources in Korean adults and that dietary As exposure may be associated with individual dietary habits and environmental As contamination among countries.