In this study, the spatial and temporal variations in the levels of C8-C40 n-alkanes and 18 polycyclic aromatic hydrocarbons (PAHs) in water and sediment from Loskop Dam (Mpumalanga Province South Africa), were investigated between 2015 and 2017. In addition, their sources, which have not been well defined, were also studied over the period. This water body is sourced from a historically contaminated water body, the Olifants River, which flows through areas where a range of industrial and agricultural activities take place. Mass crocodile and fish mortalities have been recorded in this aquatic system, and contamination by organic pollutants were highlighted as a contributing factor. The total average n-alkane concentrations in water and sediments ranged from 0.574±00811 to 18.8±1.39 µg/L and 4760±243 to 30700±906 µg/kg, respectively. Similarly, PAHs were detected at total average concentrations of between 0.150±00494 and 49.8±6.86 µg/L in water and 61.6±5.95 to 2618±300 µg/kg. n-Alkane and PAH diagnostic ratios indicated a mixture of sources of these compounds, attributed to terrestrial, submerged and floating plant material, as well as petrogenic and pyrogenic combustion. Inlet, middle and upper segment site clustering was observed with non-metric multidimensional scaling (NMDS) and hierarchical cluster analysis (HCA), mainly driven by the prevalence of PAHs at the inlet sites and n-alkanes in the upper reaches. By using indicator compounds, the sources of contamination could be predicted. The strategy described here can be applied to any water body for continuous long-term monitoring of pollutant levels and to identify sources attributing to water pollution.