Ab initio molecular dynamics (AIMD) simulations are used to calculate select thermophysical and thermodynamic properties of NaCl, UCl3 and NaCl-UCl3 molten salts. Following established approaches, the AIMD simulations include a model for Van der Waals interactions. The Langreth & Lundqvist (vDW-DF2), DFT-D3, and density-dependent energy correction (DFT-dDsC) dispersion models are first tested for molten NaCl in order to assess their accuracy for density and heat capacity predictions across a range of temperatures. Based on the NaCl results, the vdW-DF2 and DFT-dDsC methods are extended to the UCl3 system and compared to available experimental data. Next, mixtures of NaCl-UCl3 are investigated and analyzed with respect to the deviation from ideal solution behavior. For the DFT-dDsC simulations, density deviates by up to 2% from an ideal mixture, with the maximum occurring close to the eutectic composition. The mixing energy also deviates from an ideal solution and exhibits a minimum of about -0.074 to eV per formula unit, again close to the eutectic composition. Finally, the compressibility and species diffusivity of the pure and mixed salt systems are calculated. The diffusivities are slightly reduced in the mixed compared to the pure systems and the compressibilities loosely follow a linear correlation as a function of the UCl3 composition. The trends observed for mixing properties are rationalized by correlating them to the coordination chemistry, which emphasizes the importance of maintaining the extended network formed by U and Cl ions as the NaCl concentration increases. The concentration at which breakdown of the extended network occurs, roughly coincides with the minimum of both the mixing energy and the deviation from ideal solution behavior for density.