Evaluation of the hydrogeochemical processes governing the heavy metal distribution and the associated health risk is important in managing and protecting the health of freshwater resources. This study mainly focused on the health impacts due to the heavy metals pollution in a known Cretaceous-Tertiary (K/T) contact region (Tiruchinopoly, Tamilnadu) of peninsular India, using various pollution indices, statistical, and geochemical analyses. A total of 63 samples were collected from the hard rock aquifers and sedimentary formations during southwest monsoon and analysed for heavy metals, such as Li, Be, Al, Rb, Sr, Cs, Ba, pb, Mn, Fe, Cr, Zn, Ga, Cu, As, Ni, and Co. Ba was the dominant element that ranged from 441 to 42,638 μg/l in hard rock aquifers, whereas Zn was the major element in sedimentary formations, with concentrations that ranged from 44 to 118,281 μg/l. The concentrations of Fe, Ni, Cr, Al, Cr, and Ni fell above the permissible limit in both of the formations. However, the calculated heavy metal evaluation index (HEI), heavy metal pollution index (HPI), and the degree of contamination (Cd) parameters were higher in the sedimentary formation along the contact zone of the K/T boundary. Excessive health risks from consumption of contaminated groundwater were mostly confined to populations in the northern and southwestern regions of the study area. Carcinogenic risk assessment suggests that there are elevated risks of cancer due to prolonged consumption of untreated groundwater. Ba, Sr, and Zn were found to be geochemically highly mobile due to the partitioning between the rock matrix and groundwater, aided by the formation of soluble carbonato-complexes. Factor analysis indicates that the metals are mainly derived from the host rocks and anthropogenic inputs are relatively insignificant. Overall, this study indicated that groundwater in K/T contact zones is vulnerable to contamination because of the favorable geochemical factors. Long-term monitoring of such contact zones is required to avert the potential health hazards associated with consumption of the contaminated groundwater.