Anomalous concentration of Uranium in groundwater has been identified around Virakkal, Veerapanpalayam, Pakkanadu, Erithottam, Kammampatti, Kumarappalyam, Idappadiand Moolakkadu areas in parts of Salem district, Tamil Nadu. In this study, an area of 970 sq. km from Mettur in the north to Kumarapalayam in the south parallel to the Koratti shear zone has been examined for uranium content in groundwater. Systematic sampling of groundwater (n=78) from bore well, open well and hand pump have been collected. The samples were analysed for uranium concentration using LED Fluorimeter. Analysis resulted higher concentration of uranium along the southern extension of Koratti Shear Zone where the emplacement of younger granites, syenite and carbonatites has been reported. These lithounits might have played a vital role in the contribution of uranium to the groundwater. Based on the result, two areas have been identified such as North Block and South Block for detailed investigation.58 systematic samples from North block and 52 samples from South block have been collected and analysed. Uranium values assayed in these areas are many times higher than the prescribed limit of World Health organisation and Atomic Energy Regulatory Board of 30ppb and 60ppb respectively. In northern block, among 58 samples 18 samples were assayed higher than 30ppb in which the samples from Veerappanpalayam assayed upto 545.81 ppb. Apart from Veerappanpalayam, many areas such as Mosakumarapalayam (273.90), Arasiramani (250.49ppb), Vellarivalli (131.32ppb), Kodarapalayam (106.52ppb), Savuthanur (174.79ppb), Veerapanpalayam-2 (373.43ppb) and Kotamppalayam (100ppb) were assayed more than 100ppb. Similarly, in the southern block, 52 samples were assayed in which 15 samples were higher than the prescribed limit in which Kuppampatti analyzed 402.29ppb, Virakkal and Thannikuttampatti assayed more than 100ppb. Among the total samples (n=188), 28% of samples were falling under non-potable category. The Present study has spatially brought to light significant areas where groundwater enriched by uranium concentration. It is also provided indirect evidences for uranium exploration in the study area.