Résumé : Lebanon is situated in a Mediterranean semi-arid region rich in hydraulic resources but strongly under the impact of anthropogenic pressure, mainly after the industrial boost in the last 50 years. In this thesis our research is devoted to the study of water resources and the assessment of soil pollution in two contrasting watersheds that may resemble similar regions in the world. Rivers act as a collective funnel of contaminants derived from rock weathering, industrial, agricultural and urban practices. Thus we focus our study on the two main contrasting watersheds in Lebanon: an industrially dominated watershed located northwest of the country on the Mediterranean coast (Al Jouz basin), and a rural historically agricultural watershed that lies in the continental valley between the two mountainous chains (Litani basin). Geochemical analysis coupled to multi-isotopic applications was used as tools to investigate the collective influence of land-use cover, geomorphological processes, topography, soil type, geology, geography, orography, climate, and hydrological variability on drainage basin evolution. A two-year sampling strategy was followed (2011-2013) to collect not only water samples at various depths in the reservoir and in the piezometers, but also sediments (lacustrine, riverine and coastal) and soils (surficial and cores) to cover seasonal variations (rainy, first flush and dry seasons) in both studied areas. The results highlight the entire mechanism of characterization, origin, and partitioning between the dissolved and particulate phases of pollutants. Furthermore, the environmental implication of the Qaraaoun reservoir was assessed by emphasizing water hydrodynamics and its interaction with the watershed. Characterizing industrial and agricultural pollution allows the understanding of metal behavior and the prediction of its fate, in association with the environmental receiving media in semi-arid and Mediterranean areas. This work was the first to trace pollution sources and to reconstruct the metal fluxes in two of the most environmentally significant watersheds in the country. Stable and radioactive Pb isotopes were used in addition to 137Cs to study the geomorphological influence and the chronology of the environmental stress exerted by the factory and the dam on basin ecology. Moreover, the nature of the Qaraaoun reservoir and the internal hydrological dynamics were explored using stable hydrogen and oxygen isotopes to delineate the reservoir water layers and its fast response to meteorological and hydrodynamic changes in the watersheds, and to demonstrate its strong hydrological connectivity with groundwater. Reservoir water balance was made, indicating groundwater influx into the reservoir which was reported for the first time. The water hydrodynamics was also assessed using a box model, which in its role can be used to evaluate the reservoir water balance and hydro-project functionality and to establish the basis for water sustainability in the long term. This work has yielded a better understanding of biogeochemical processes under different environmental conditions. The treated issues in this thesis will provide a foundation for future hydropower projects and allow one to draw a road-map for national management plans, and to raise the alert for remediation processes and management methods to preserve the environment and resource sustainability, and ultimately the wellbeing of the local population.