Groundwater is a vital resource for drinking and agricultural needs globally, yet its quality is increasingly threatened by anthropogenic activities. This chapter investigates the health risks associated with heavy metal contamination in the coastal aquifers of KwaZulu-Natal, South Africa, a region reliant on groundwater for agriculture and domestic use. Employing a multidisciplinary approach, 128 groundwater samples were analyzed for metals such as Cd, Pb, Cr, and Zn. Source apportionment via Positive Matrix Factorization (PMF) identified agricultural fertilizers (e.g., phosphate-based inputs) and industrial activities as primary contamination sources. Probabilistic health risk assessment, integrated with Monte Carlo simulations, quantified non-carcinogenic and carcinogenic risks for adults and children. Results revealed elevated risks, particularly for children, with cadmium and chromium posing significant carcinogenic threats. Spatial mapping highlighted contamination hotspots in southern and central regions, underscoring the urgency for targeted mitigation strategies. The study bridges hydrochemical data with public health insights, offering actionable recommendations to align groundwater management with sustainable development goals.