To address the imbalance in energy supply and demand across different regions and seasons, the thermochemical conversion process was selected to efficiently utilize surplus energy. In the search for suitable novel materials, this study developed a porous matrix “in-salt” composite using a carbonized metal-organic framework as the carrier and LiCl as the primary reactant. When exposed to water vapor, the innovative material enabled both adsorption and desorption of water vapor, leading to the release and storage of thermal energy, thereby achieving effective energy storage. Using Zn(NO₃)₂·6H₂O and Co(NO₃)₂·6H₂O as metal ion sources and 2-methylimidazole as the ligand, bimetallic zeolitic imidazolate frameworks (BMZIFs) were fabricated via the liquid-phase precipitation method. The composite specimen prepared at a carbonization temperature of 1000 °C with a 20% LiCl mass concentration exhibited the most promising thermal storage performance, achieving the highest capacity, with a final water loss of 53.56% and a stable water adsorption capacity of about 0.831 g·g⁻¹.