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Abstract: Elevated As concentrations in groundwater of the Huhhot basin (HB), Inner Mongolia, China, and the western Bengal basin (WBB), India, have been known for decades. However, few studies have been performed to comprehend the processes controlling overall groundwater chemistry in the HB. In this study, the controls on solute chemistry in the HB have been interpreted and compared with the well-studied WBB, which has a very different climate, physiography, lithology, and aquifer characteristics than the HB. In general, there are marked differences in solute chemistry between HB and WBB groundwaters. Stable isotopic signatures indicate meteoric recharge in the HB in a colder climate, distant from the source of moisture, in comparison to the warm, humid WBB. The major-ion composition of the moderately reducing HB groundwater is dominated by a mixed-ion (Ca–Na–HCO3–Cl) hydrochemical facies with an evolutionary trend along the regional hydraulic gradient. Molar ratios and thermodynamic calculations show that HB groundwater has not been affected by cation exchange, but is dominated by weathering of feldspars (allitization) and equilibrium with gibbsite and anorthite. Mineral weathering and mobilization of As could occur as recharging water flows through fractured, argillaceous, metamorphic or volcanic rocks in the adjoining mountain-front areas, and deposits solutes near the center of the basin. In contrast, WBB groundwater is Ca–HCO3-dominated, indicative of calcite weathering, with some cation exchange and silicate weathering (monosiallitization). [Copyright &y& Elsevier]