Geogenic or naturally occurring arsenic (As) contamination of groundwater is widespread particularly in south-east Asian countries (Kumar et al., 2016a; Mandal and Suzuki, 2002; Naidu et al., 2007; Singh et al., 2016). It has a significant threat to human health and a massive challenge to clean water supplies in the affected areas. Recent estimate shows ∼150 million people are affecting around the world via groundwater extracting from naturally occurring As-contaminated aquifers (Podgorski et al., 2017). Our research is focused on the central Gangetic Basin located in the states of Uttar Pradesh and Bihar in India, is a highly populated and extremely fertile area (Saha and Sahu, 2016). The area of central and upper Gangetic Basin (∼0.25 million km2), ranges from the Garo Rajmahal Hills in the south to the Tarai zone in the north, covers much of Bihar and Uttar Pradesh, India population: ∼303.9 million (Chandramouli and General, 2011; Saha and Sahu, 2016). We have applied a holistic approach to understand the mobility of inorganic As species (AsIII and ASV) in water, soil-sediments and plants products (grains). We have identified the As-hot spots and estimated health risk on the consumption of contaminated water and food on the residing people.