This work describes a material that has improved mechanical and reactivity properties for use in thermochemical energy storage systems based on CaO/Ca(OH)2 reversible reactions. The composite material uses sodium silicate as a binder of active CaO particles. The observed mechanical stability of the material is due to the formation of hard Ca silicates resulting from the reaction of the binder with the exterior of the CaO particles. A screening of the main synthesis variables affecting the composite was carried out, including Ca precursors of different particle size, a range of molar Ca/Si ratios, as well as the curing and calcination conditions. The most suitable material (containing CaCO3 with a particle size of 36–63 μm as calcium precurs...