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Arsenic is a toxic element widely spread in soils and groundwater that can cause a great hazard to ecology and human health. In this paper, 51 groundwater and 12 sediment samples were analyzed to investigate the sources and evolution mechanism of arsenic and identify the hydrochemical characteristics of groundwater in Hetao Plain, Inner Mongolia through Kriging interpolation, Piper trilinear diagram and ion correlation analysis. Results show that high arsenic groundwater is mainly distributed in the areas with reducing environment. Arsenic has a strong positive correlation with bicarbonic acid and a negative correlation with nitric acid. Arsenic in the sediment is easily adsorbed by iron-manganese compounds. In a reducing environment, arsenic is however released while iron-manganese oxides are reduced. Through triangular fuzzy numbers, a health risk assessment was conducted to evaluate the hazard caused by high arsenic groundwater to humans. Results suggest that the highest carcinogenic risk values of arsenic for children, men, and women are 3.9 × 10−3, 2.38 × 10−3, and 2.35 × 10−3, respectively that greatly exceeds the acceptable risk value. The findings of this paper provide useful insight into the occurrence mechanism of arsenic in those areas with high arsenic groundwater and the potential health risk to humans. • Genetic interpretation of high Arsenic in groundwater is presented. • Interactive processes between groundwater ions and As is interpreted. • Health risk assessment is performed with triangular fuzzy theory. [ABSTRACT FROM AUTHOR]