The growing population, pollution, and misuse of freshwater worldwide necessitate developing innovative methods and efficient strategies to protect vital groundwater resources. This need becomes more critical for arid/semi-arid regions of the world. The present study focuses on a GIS-based assessment and characterization of groundwater quality in a semi-arid hard-rock terrain of Rajasthan, western India using long-term and multi-site post-monsoon groundwater quality data. Spatio-temporal variations of water quality parameters in the study area were analyzed by GIS techniques. Groundwater quality was evaluated based on a GIS-based Groundwater Quality Index (GWQI). A Potential GWQI map was also generated for the study area following the Optimum Index Factor concept. The most-influential water quality parameters were identified by performing a map removal sensitivity analysis among the groundwater quality parameters. Mean annual concentration maps revealed that hardness is the only parameter that exceeds its maximum permissible limit for drinking water. GIS analysis revealed that sulfate and nitrate ions exhibit the highest (CV > 30%) temporal variation, but groundwater pH is stable. Hardness, EC, TDS, and magnesium govern the spatial pattern of the GWQI map. The groundwater quality of the study area is generally suitable for drinking and irrigation (median GWQI > 74). The GWQI map indicated that relatively high-quality groundwater exists in northwest and southeast portions of the study area. The groundwater quality parameter group of Ca, Cl, and pH were found to have the maximum value (6.44) of Optimum Index factor. It is concluded that Ca, Cl, and pH are three prominent parameters for cost-effective and long-term water quality monitoring in the study area. Hardness, Na, and SO(4), being the most-sensitive water quality parameters, need to be monitored regularly and more precisely.