Elemental sulfur provides a low-cost, high-performance thermal storage option for a wide range of applications and over an exceptionally wide range of temperatures (50 °C to over 600 °C). In previous efforts we have shown impressive performance for 200–600 °C, while in this study we examine the low-temperature (50–200 °C) thermal charge and discharge behavior of isochoric sulfur-based storage using a detailed computational model solving for the conjugate heat transfer and solid-liquid phase change dynamics. The model provides excellent agreement with experimental results. We show that sulfur exhibits lower viscosity because of reduction in the chain-length of polymeric sulfur caused by trace amounts of organic substances resulting in attractive charge and discharge performance. The results from the parametric analysis of pipe diameter on the charge and discharge heat transfer characteristics are used to develop a simple, generalized correlation that relates the transient sulfur temperature and liquid fraction evolution as a function of dynamically evolving buoyancy-Fourier number due to the solid-liquid phase change. This solid-liquid buoyancy-Fourier, BFs-l, correlation can be used for effectively designing sulfur-based thermal energy storage systems for transient operation in low temperature applications.