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Groundwater samples (n = 152) were collected in the Thar Desert of the Umarkot Sub-District, Pakistan to evaluate the geochemical controls on the occurrence of high fluoride (F-) levels within the study area. Fluoride concentrations range from 0.06 to 44.4 mg/L, with mean and median values of 5.22 and 4.09 mg/L, respectively; and roughly 84% of the samples contain fluoride concentrations that exceed the 1.5 mg/L drinking water standard set by WHO. The overall groundwater quality reflects the influences of silicate mineral weathering and evaporation. Fluoride originates from the weathering of minerals derived from Type-A granite and possibly anion exchange (OH- for F-) on clays and weathered micas under high pH conditions. High fluoride levels are associated with Na-HCO3 type water produced by calcite precipitation and/or base ion exchange. Depleted calcium levels in groundwater allow higher fluoride concentrations to occur before the solubility limit for fluorite is reached. (C) 2015 Elsevier B.V. All rights reserved.