Molten Salt Reactors (MSRs) are envisioned as a potential pathway to safer, more economical nuclear electricity generation and supply of industrial heat. MSRs under consideration today are either solid-fueled salt-cooled designs or liquid-salt-fueled designs with chloride or fluoride based salts. A significant knowledge gap exists in the data for the fundamental properties relevant to fuels and coolants for MSRs that needs to be addressed in order to expedite the technical readiness level of the MSR design concepts. With the rapid development and improvement of computational materials science, computational methods such as Density Functional Theory (DFT) calculations and ab initio Molecular Dynamics (AIMD) simulations are widely used as an effective and reliable tool to investigate the atomic interaction in materials. In this article, the density of the LiCl-KCl system was determined via AIMD calculations and verified using new experimental analyses. AIMD was further utilized to calculate the compressibility, heat capacity, enthalpy of mixing, and Gibbs free energy of mixing. This work spans a wider range of compositions and temperatures than have previously been explored computationally for this pseudo-binary system and provides the basis for further advanced thermophysical property evaluation utilizing AIMD methods.