The Olifants River catchment has been adversely affected by anthropogenic land-use activities over the last decade. This study aims to determine the variation in surface and groundwater concerning heavy metal pollution. The collection of surface and groundwater was performed at three different land-use locations, namely, wastewater treatment works effluent (WWTW), acid mine drainage effluent (AMD), and borehole water (B·H.). These locations were located in the Mpumalanga and Limpopo provinces of South Africa. A total of 15 samples, five from effluent and water samples, were collected during the summer (October 2019). Several parameters were measured to see if the effluent and water was safe for drinking and irrigation purposes. The values of pH and Turbidity were within the permissible limit of the South African guidelines, while electric conductivity exceeds the limit. The samples were analyzed for heavy metals using the inductively coupled plasma-mass spectroscopy process. The results revealed that Cu, Ni, Zn, and Ba were all within the South African National Standards prescribed by the Department of Water and Sanitation's drinking and irrigation limits. At the same time, Fe and Mn exceeded the limit. The metals concentrations observed were non-significant (p > 0.05). The data obtained were used for statistical analysis and applying a heavy metal pollution index (HPI) and metal index (MI). Analysis of variance showed that all metals, Cu, Fe, Ni, Mn, Zn, and Ba, express statistically significant values (p < 0.05). The Heavy metal pollution index based on six selected heavy metals indicated that more than 75% of the area does not have good water quality, whereas less than 35% was suitable. However, these values at all stations were below the critical importance of 100. Furthermore, this study highlights that infants, children, and adults consuming water from the contaminated boreholes were exposed to significant amounts of metals. However, the health risk index values of less than 1 indicate a relative absence of health risks associated with the consumption of contaminated water. The health risk assessment like chronic daily intake (CDI) and hazard quotient (H.Q.) was calculated based on heavy metal concentrations. The values for CDI were found in the order of Ba > Zn > Ni > Cu and Fe for infants, children, and adults, and the values for heavy metals in water samples indicating no health risk.