The chronological and spatial relationships between tectonic faulting and magmatic activity of the Earth’s crust within the western part of the Ukrainian Shield during the Paleoproterozoic (2.08–1.73 Ga) was investigated. Based on tectonophysical analysis of major fault zones (e.g., Sushchany–Perha, Nemyriv, Khmilnyk, Zvizdal–Zalissia, Brusyliv) and on structural analysis of the Novohrad-Volynskyi granitoid massif and the Korosten Pluton of gabbro–anorthosite and rapakivi granite was delineated discrete stages of tectono-magmatic activity. These stages were accompanied by changes in the regional stress–strain regime and the formation of distinct magmatic complexes. Results of 3D gravity modelling reveal two dominant fault systems – northeast-trending and sub-latitudinal – that control the distribution of structural heterogeneities in the crust. The meridional Bilokorovychi fault zone is established as a structural boundary dividing the western Ukrainian Shield into two parts: western and eastern. Both differ significantly in different density and magnetic properties, as well as in the thickness of the crust. The western part is characterized by thicker crust (up to 60 km), positive regional magnetic anomalies achieving values up to +350 nT and higher densities on Moho (up to 3.12 g cm⁻³). On the other hand, the eastern part is represented by thinner crust (only 40–50 km), mostly negative magnetic anomalies, which in the space of Korosten Pluton reach values of −350 nT and lower values of the densities on the Moho (2.98–3.06 g cm⁻³). The data highlight the central role of tectonic faults in building the present crustal structure, reflected in the patterns of the regional magnetic field and in crustal density heterogeneity.