TiS2 is a stable layered transition metal sulfide with applications in energy storageEnergy storage, electronic devices, and catalysis. Synthesis methods include colloidal synthesis, liquid-phase reaction, and low-temperatureTemperature chemical precipitation, but these often introduce impurities and have low reproducibility and low productivity. The CVT method, using a completely enclosed environment, significantly reduces impurity introduction, resulting in high-purity and well-crystallized products. This study synthesized TiS2 by the CVT method, examining the effects of Ti/S stoichiometric ratio, calcination temperatureTemperature, and reaction time on the product's structure and morphologyMorphologies. Optimal conditions were found to be a Ti/S ratio of 1:2, a calcination temperatureTemperature of 600 °C, and a calcination time of 24 h. Crystalline products are difficult to obtain below 500 °C or with a Ti/S ratio of 1.5. With the increase of reaction time, TiS2 shows better crystallinity and homogeneity. TiS2 synthesized by the CVT method exhibits a maximum specific capacity of 225 mAh g−1 at a current densityDensity of 50 mA g−1 and retains 60.8% capacity after 10,000 cycles at 1 A g−1.