A study has been carried out in crystalline hard rock aquifers of Madurai district, Tamil Nadu, to identify the spatial and temporal variations and to understand sources responsible for hydrogeochemical processes in the region. Totally, 216 samples were collected for four seasons [premonsoon (PRM), southwest monsoon (SWM), northeast monsoon (NWM), and postmonsoon (POM)]. The Na and K ions are attributed from weathering of feldspars in charnockite and fissile hornblende gneiss. The results also indicate that monsoon leaches the U ions in the groundwater and later it is reflected in the (222)Rn levels also. The statistical relationship on the temporal data reflects the fact that Ca, Mg, Na, Cl, HCO3, and SO4 form the spinal species, which are the chief ions playing the significant role in the geochemistry of the region. The factor loadings of the temporal data reveal the fact that the predominant factor is anthropogenic process and followed by natural weathering and U dissolution. The spatial analysis of the temporal data reveals that weathering is prominent in the NW part and that of distribution of U and (222)Rn along the NE part of the study area. This is also reflected in the cluster analysis, and it is understood that lithology, land use pattern, lineaments, and groundwater flow direction determine the spatial variation of these ions with respect to season.