An effort has been made, perhaps for the first time, to elucidate the concentration of arsenic (As) in soil-rice plant systems in the Bashkandi Block of Barak Valley in Assam, Northeastern India. The present study found that the concentration of As in groundwater is much higher than the WHO permissible limit (10 μg/L) and ranges from 12 to 310 μg/L, and the level of concentration in the soil varies from 5.7 to 12.4 mg/kg. Chemical extraction and its analysis of As in the soil indicate that the pool of As is predominantly associated with organic matter and amorphous Fe-oxides and weakly associated with mobile fractions and loosely bounded As present in the soil. In addition, the extraction result shows a significant amount of As associated with pyrite. The rice plant analysis reveals that the concentration of As content ranges as follows: in grain, 0.9 to 1.51 mg/kg, followed by the husk, 1.1 to 1.35 mg/kg; straw 0.82 to 1.45 mg/kg and 8.2 to 57.9 mg/kg in the root. The root of the rice plant accumulated high amounts of As, followed by straw, husk, and grain. The correlation coefficient calculations indicate the pathway of As translocation along with Fe and S from the soil to the rice grain. The most prominent finding of this work is that the As concentration has a direct entry into the human food chain, and the population in the area seems to be exposed to As toxicity by ingestion of groundwater and rice.