Abstract: Hydrogeological and geochemical data, in conjunction with the results of an electrical imaging tomographic survey, were examined to determine the main factors and mechanisms controlling the groundwater chemistry and salinity of the unconfined aquifer of Bou-Areg, on the Mediterranean coast of NE Morocco. In addition, statistical and geochemical interpretation methods were used to identify the distribution of the salinity. Multivariate statistical analysis (cluster and principal component factors) revealed the main sources of contamination. Groups A, B, and C in the cluster analysis and Factors 1–3 (Factor 1: CE, Cl−, K+, SO42-, and Mg2+; Factor 2: Ca2+, HCO3-, and pH; Factor 3: NO3-) represent the ‘signature’ of seawater intrusion in the coastal zone, the influence of marly-gypsum outcrops in the upstream zone, and anthropogenic sources, respectively. The ionic delta, the ionic ratio, the saturation index, and Stuyfzand’s method were applied to evaluate geochemical processes. The results obtained indicate, on the one hand, the phenomenon of salinization in both the coastal and the upstream zones, and on the other, the dilution of groundwater by recharge. Cation exchange is shown to modify the concentration of ions in groundwater. Locally, with respect to salinization processes in the coastal zone, the results of electrical imaging tomography show that salinity increases both with depth and laterally inland from the coastline, due to seawater intrusion.