This chapter focussed on assessing the geochemical characteristics and quality of groundwater in the eastern coastal aquifers of South Africa such as Maputoland, uMhlathuze, and Tugela to determine its suitability for domestic, agricultural, and industrial uses. Given the agricultural dominance in the region, understanding groundwater quality is crucial for sustaining soil productivity and public health. These physico-chemical, ionic data were used to compute various hydrochemical indices such as Water Quality Index (WQI), Sodium Percentage (%Na), Kelly’s Ratio, Magnesium Hazard, Sodium Adsorption Ratio (SAR), Permeability Index, and Corrosivity Ratio, following standard procedures and using WHO and SANS guidelines. Spatial variation was mapped to identify zones of concern. The results indicated spatial differences in groundwater chemistry, with elevated salinity and contamination levels in the central and southern aquifers. The chapter provided a comprehensive evaluation groundwater suitability and highlighted the importance of regular monitoring to inform sustainable water management in coastal agricultural regions.