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Groundwater is a major source of water supply for domestic and irrigation uses in semiarid, remote but rapidly developing Kilasaifullah district part of Zhob River Basin, located at PakistanAfghanistan Border. Zhob River is among few major rivers of perennial nature in Balochistan, which flows from WSW to ENE and falls in Gomal River, a tributary of Indus River. Keeping in view the important geopolitical position and rapid development of the region, this study is primarily focused on groundwater chemistry for contamination sources as well as agriculture development. Water samples from open and tube wells are analyzed and calculated for electrical conductivity (EC), total dissolved solids (TDS), turbidity, pH, K+, Na+, Ca2+, Mg2+, HCO?3-, Cl-, NO?3-, SO?42-, PO?43-, sodium percent (Na%), sodium adsorption ratio (SAR), Kelly’s index (KI), and heavy metals (Fe, Cu, Cr, Zn, Pb, and Mn). On the basis of the chemical constituents two zones within the study area are identified and possible causes of the contaminants are pointed out. Two recharge areas were responsible for the different chemical results in groundwater, e.g., zone A was recharged from NNW saline geological formations (Nisai, Khojak, Multana, Bostan formations, and Muslim Bagh ophiolites), which are concentrated with high sodium and chloride. On the other hand Zone B was sourced from SSW from carbonate rich rocks (Alozai, Loralai, Parh formations, and Muslim Bagh ophiolites). The groundwater is classified as C2S1, C3S1, C3S2, C4S2 on the basis of EC and SAR values which indicate that most of the water of both zones can be used for irrigation safely except the samples plotted in C3S2 and C4S2 categories which could be dangerous for soil and crops. Groundwater samples are plotted in good to permissible limits with some samples excellent to good and few samples belong to doubtful category based on sodium percent. Groundwater of zone A is unsuitable for irrigation use due to higher values of KI (more than one) but water of zone B are good for irrigation based on KI. In general, water of both zones is suitable for irrigation but care should be taken during the selection of crops which are sensitive to alkalinity or sodium hazards particularly in zone A.