From a public health perspective, the monitoring of water quality intended for human consumption belongs to the operational and audit management of the supply zones. Our study explores the spatial and temporal patterns of the parameters of drinking water in Sibiu County, Romania. We related the relevant physical-chemical parameters (ammonia, chlorine, nitrates, Al, Fe, Pb, Cd, Mn, pH, conductivity, turbidity, and oxidizability) and radioactivity (gross alpha activity, gross beta activity, and radon-222 content) from a 5-year survey to the water source (surface water and groundwater, which may be of subsurface or deep origin), space (sampling locality) and time (sampling month and year). We conducted a combined evaluation using the generalized linear mixed models (GLMMs), Pearson correlation analysis of the physical-chemical parameter, multivariate linear redundancy analysis (RDA), t-value biplots construction, and co-inertia analysis. The obtained regional model shows that the source, locality, and month of sampling are significant factors in physical-chemical parameters’ variation. Fe and turbidity have significantly higher values in surface water, and nitrates and conductivity in groundwater. The highest values are recorded in January (nitrates), March (Cl, ammonia, pH) and August (Fe, turbidity). The RDA ordination diagram illustrates the localities with particular or similar characteristics of drinking water, two of which (rural sources) being of concern. The water source is the best predictor for radioactivity, which increases from surface to ground. The gross alpha and beta activities are significantly and positively correlated, and are both correlated with conductivity. In addition, the gross alpha activity is positively correlated with nitrates and negatively with pH, while the gross beta activity is positively correlated with Mn and negatively with Fe; these relationships are also revealed by the co-inertia analysis. In conclusion, our model using multilevel statistical techniques illustrates a potential approach to short-term dynamics of water quality which will be useful to local authorities.