In this study, we performed a numerical investigation of the thermophysical properties of liquid (U, Zr) mixtures, which are particularly relevant in the context of hypothetical nuclear accidents and the formation of in-vessel coriums. To do so, atomistic simulations leveraging classical molecular dynamics and an interatomic potential developed for solid (U, Zr) structures are performed. Our methodology is first validated by comparing the predictions of our model for the melting temperature and the structure factors to experimental, phase diagram, and ab initio data. We then use the approach to evaluate the temperature and composition dependence of four fundamental properties in the context of coriums: density, heat capacity, compressibility, and viscosity. Systematic comparisons to the existing experimental data are performed and discussed. In particular, the viscosity of liquid (U, Zr) mixtures is investigated by comparing diffusion calculations and the Stokes–Einstein formula as well as the results obtained with the Green–Kubo methodology, empirical predictions, and experimental data. Notably, the viscosity of the mixtures is predicted to be significantly higher than that of the single-element liquids, which is unexpected and could have crucial consequences on the early stages of the formation and flow of in-vessel corium.