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Background: Arsenic toxicity in humans is well recognized. It has been classified as a class I human carcinogen by the International Agency of Research on Cancer. Arsenic enters the human body mainly through drinking water, dermal contact, food chain, and inhalation. The Gangetic belt of India is considered as one of the most arsenic-affected sites in India. Health risk assessment of the human population exposed to arsenic in drinking water is important. The present study was conducted to assess the groundwater quality and associated health risks on the people of Samastipur district in the middle Gangetic belt of Bihar. Groundwater samples from 40 different study sites were collected and analyzed for various physico-chemical properties of water. Results: Arsenic (> 0.01 mg/L) was present in 33% of the water samples analyzed. Subsequently, an assessment for carcinogenic risk and non-carcinogenic health risk (HQ) for children, females, and males in the study area was performed. Risk assessment showed that 100% of the population may be at carcinogenic health risk and 35% may be at non-carcinogenic health risk, and among these, children were at maximum risk. Furthermore, the computational assessment of the arsenic–protein interactome revealed the enrichment of cancer-related pathways. Conclusions: It is recommended to provide arsenic-free alternate sources of water in the study area. [ABSTRACT FROM AUTHOR]