To elucidate the physicochemical properties of the artificial silicate composite material, K-feldspar and lime were reacted in mild hydrothermal conditions (different reaction temperatures and various K-feldspar/lime ratios). Formed phases were investigated using various techniques, such as X-ray powder diffraction, the Rietveld method, scanning electron microscopy (SEM), and inductively coupled plasma-optical emission spectrometry. The analysis revealed that tobermorite, grossular (hydrogarnet), alpha-dicalcium silicate hydrate (α-C2SH), amorphous calcium silicate hydrate, potassium carbonate, bütschliite, calcite, and calcium hydroxide formed with various conditions. Both the temperature and the Ca/Si molar ratio in the starting material greatly affected the formation of phases, especially the generation of tobermorite and α-C2SH. The substitution of H4O4 ↔ SiO4 proceeded with the increase of the Ca/Si molar ratio rather than the reaction temperature and the reaction time. More hydrogen was incorporated in hydrogarnet through the substitution of H4O4 ↔ SiO4 with the increase of the Ca/Si molar ratio in the starting material. Due to the properties of tobermorite as a cation exchanger and its potential applications in hazardous waste disposal, experimental parameters should be optimized to obtain better performance of the artificial silicate composite material from K-feldspar and lime hydrothermal reaction. The dissolution mechanism of K-feldspar was also discussed.