This paper investigates the thermal battery as a research topic. We conducted an in-depth analysis of various thermal battery aspects, such as the cathode material CoS2 and electrolyte material morphology, crystal type, and interface state changes before and after service. The aim was to explore the core reaction and main failure mechanisms of the thermal battery. Prior to the reaction, the thermal battery cathode and electrolyte material consisted of pure-phase CoS2 and a composition of MgO-LiF/LiBr/LiCl. After service, the cathode and electrolyte of the single thermal battery exhibited significant morphological alterations caused by the presence of a molten state. The cathode transformed from CoS2 to Co3S4 and Co9S8 together with the presence of a marginal quantity of Co monomers visible throughout the discharge process, which was confirmed by means of XRD and XPS analyses. After the reaction, the electrolyte material was primarily made up of LiF, LiBr, and LiCl while the crystal components remained largely unaltered, albeit with apparent morphological variations. As was deduced from the thermodynamic analysis, the cathode material’s decomposition temperature stood at 655 °C, exceeding the working temperature of the thermal battery (500 °C) by a considerable margin, which is indicative of outstanding thermal durability within the thermal battery’s operational temperature range. Furthermore, the discharge reaction of the positive electrode was incomplete, resulting in reduced CoS2 residue in the thermal battery monomer after service. The reaction yielded a combination of Co3S4, Co9S8, and small amounts of Co monomers, indicating possible inconsistencies in the phase composition of the pole piece during the reaction process. In this study, we examine the distribution of residual stress in the thermal battery under various operating conditions. The simulation results indicate that exposure to a 70 °C environment for 2 h causes the maximum residual stress of the battery, which had an initial temperature of 25 °C, to reach 0.26 GPa. The thermal battery subjected to an initial temperature of 25 °C exhibited a maximum residual stress of 0.42 GPa subsequent to a 2-hour exposure to a temperature of −50 °C.