To clarify the groundwater-soil-crop relationship with respect to arsenic (As) contamination, As concentration was measured in tubewell (TW) water, surface soil from farmyards and paddy fields, and fresh taro (Colocasia esculenta) leaves from farmyards in the farming villages of Bangladesh. The As concentration in TW water from farmyards was at least four times higher than the Bangladesh drinking water standard, and the concentration in fresh taro leaves was equal to or higher than those reported previously for leafy vegetables in Bangladesh. As concentration of surface soils in both farmyards and paddy fields was positively correlated with that of the TW water. Further, the concentration in surface soil was positively correlated with levels in fresh taro leaves in the farmyard. This study, therefore, clarified the groundwater-soil-crop relationship in farmyards and the relationship between groundwater-soil in paddy fields to assess the extent of As contamination in Bangladeshi villages.