Fine-grained sedimentary deposits can bear an increased risk for building settlements due to their moderate stiffness and strength properties, as well as high groundwater tables. However, some buildings, e.g., situated on shallow foundations in Alpine basins, show only relatively small settlements because the formation of carbonate cement can create bridging bonds between the detrital soil particles, leading to increased stiffness. These weak bonds can be damaged through dynamic loads and high static loads, causing a weakening of the soil’s microstructure and resulting in large settlements in several cases. However, the environmental controls and mechanistic processes underlying the formation versus damaging of microstructure in fine-grained, postglacial sediments are, to date, poorly understood. In the present study, fine-grained sediments are artificially cemented by calcium carbonates (CaCO3) to investigate (i) the influence of a mild and sustainable cementation process on the stress–strain behavior of silicate- and carbonate-rich soils and (ii) the possibilities and limitations of artificial microstructure development for soil stabilization. Incremental load oedometer testing (IL), bender element testing (BE), X-ray diffraction (XRD), scanning electron microscopy (SEM) and Brunauer–Emmett–Teller (BET) specific surface area (SSA) measurements are used to characterize the development of cementation and to elucidate the improvements in the soil mechanical properties. It is shown that cementation induced by CaCO3 mineralization (by 5–15% replacement) leads to an increased stiffness (factor ≈ 5–7) and shear wave velocity (factor ≈ 1.1), caused by the formation of nanocrystalline, particle-binding CaCO3 cements. The improvement of soil stiffness is dependent on the CaCO3 replacement level, reaction time and primary soil mineralogical composition.