The processed discharges from Tangier Automotive City’s (TAC) Chrafate Wastewater Treatment Plant (WWTP) contaminate the Jouamaa Hakama groundwater and the Ouljat Echatt river. We aimed to study the unknown interactions between surface water (SW) and groundwater (GW). A total of nine Jouamaa Hakama GW samples and eleven Ouljat Echatt SW samples were taken and analyzed in 2021 and 2022 to determine 16 physical and chemical parameters (pH, temperature (T), electrical conductivity (EC), dissolved oxygen (DO), total hardness (TH), turbidity (TURB), and total dissolved solids (TDS), cations: Na , K , Mg2 and Ca2 , anions: Cl−, CO32−, HCO3−, NO3−, and SO42−). For exploitation of the data, we used a methodology based on hydrochemical modeling (HM), principal component analysis (PCA), Water Quality Index (WQI), Irrigation Water Quality Index (IWQI), inverse distance weighted interpolation (IDW) using Geographic Information Systems (GIS), and regression analysis (RA). We studied the interaction of the surface water of the river (contaminated by discharges from the WWTP) with the shallow groundwater on a strip of 100 m on either side of the river to understand the transverse and longitudinal dispersion of this pollution The investigations indicated that the major ions found in GW and SW were characterized in a different order in the anion list order Cl− > CO32− > NO3− > HCO3− > SO42− and Cl− > SO42− > CO32− > NO3− > HCO3−, respectively, while the concentrations of cations showed the same order for both: Na > Ca2 > Mg2 > K . As a result, GW showed in the Piper diagram the type of sodium chloride to magnesium carbonate, while SW belongs to the sodium chloride to magnesium sulfate type. The WQI showed that the river waters are all unsuitable for use (WQI > 100), while the GW is of poor quality (WQI > 76). Moreover, the results of the GW–SW interaction along the river revealed a significant relationship (R2 = 0.85), which means that strong circulation and the infiltration of contaminated SW into shallow GW occur in this area. The approaches followed have been proven effective in evaluating water quality for human and animal uses. These results can help decision-makers in the region take suitable management measures to mitigate this environmental problem.