Aeromagnetic (AM) and Landsat Thematic Mapper (TM) data from the south-central Zimbabwe Craton have been processed for the purpose of regional structural mapping and thereby to develop strategic models for groundwater exploration in hard-rock areas. The lineament density is greater on TM than on AM images, partly due to the resolution of the different datasets, and also because not all TM lineaments have a magnetic signature. The derived maps reveal several previously undetected lineaments corresponding to dykes, faults, shear zones and/or tectonically-related joints, striking predominantly NNE, NNW and WNW. We suggest the possible hydrogeological significance of some of these patterns as follows: the aeromagnetic data can be used to map faults and fractures of considerable depth which are likely to be open groundwater conduits at depth (typically under tension), while TM lineaments, although not necessarily open (mostly under compression), represent recharge areas. The interpreted persistent lineation and well developed fracture patterns are correlated with existing boreholes and indicate a spatial relationship between regional structures and high borehole yields (> 3 m 3/h). This relationship is combined with other lithological and hydrogeological information to identify potential regional groundwater sites for detailed ground investigations. These are defined as dyke margins, faults, fractures/joints or intersections of any combination of these structures. Priority should be given to coincident AM/TM lineaments (e.g., NNW and NNE fractures) and continuous structures with large catchment areas (e.g., NNE and WNW faults). The late Archaean (2.6 Ga) granites are considered the most favourable unit because of their associated long and deep brittle fractures between numerous bornhardts (inselbergs) and kopjes. Several small-scale TM lineaments also form important local sources of groundwater for hand-dug wells. Based on measured rock susceptibilities from the area, we present a model of the typical magnetic responses from the possible groundwater exploration targets. The developed magnetic model could be applicable to similar terrains in other Archaean Cratons.