This dataset contains experimental data and scanning electron microscope (SEM) images generated during a study on the effects of surface chemistry on the mechanical consolidation of silicate-based geomaterials. The experiments were performed at Sandia National Laboratories in Albuquerque, New Mexico, under the Laboratory Directed Research and Development (LDRD) program. Data were collected to support the manuscript titled "Strengthening Effects of Surface Chemistry on the Consolidation of Silicate-Based Geomaterials" by R. C. Choens, J. Wilson, and A. G. Ilgen; the associated publication will be added to this submission once available. The dataset includes nanoindentation measurements on individual oligoclase grains under varying saturation conditions (dry, water-saturated, and Na2SO4 brine-saturated), as well as consolidation test data on both synthetic oligoclase grain packs and natural Torrey Buff sandstone. Consolidation experiments also include acoustic emission monitoring and post-deformation microstructural characterization.