This work 1) draws insights on molten salt structure and properties directly from ab initio molecular dynamics (AIMD) simulations, 2) demonstrates the advantageous symbiosis of computational and experimental collaborations on molten salt research, and 3) simultaneously generates ab initio data sets for fitting an interatomic potential model for classical molecular dynamics (MD) simulations. This work discusses the motivations for AIMD simulations of molten salts, thermophysical properties and structural characteristics of interest, advanced methodologies for AIMD simulations, and several completed AIMD studies on molten salts. Of import are the methodological contributions of this work to AIMD simulations, primarily the radical increase in generalized gradient planewave energy cutoff used to more accurately model the electron distribution across a highly-polarizable molten salt. Cutoffs of up to 2500 Rydbergs are used in this work, but 2000 Rydbergs is found to be sufficient for most AIMD NpT modelling of molten fluorides. The equilibrium liquid density of eutectic FLiNaK as a function of temperature is found to agree with the experimental density reported by Chrenkova et al. to within 0.2%, and the equilibrium liquid density of eutectic FMgNaK is found to agree with experimental measurements reported herein to within 4%. Self-diffusion coefficients in FMgNaK are also considered, with applicability to other halide salts. Molybdenum, Cesium, iodide, nickel, hydrogen, oxide, and uranium complexation are examined. It is found that solvation strength can be qualitatively determine via AIMD simulations, and that poorly solvated solutes will minimize the surface area of interaction with the salt solution. Cesium in particular is shown to be volatile or retainable in FLiBe at 500, 650, and 800 ËšC based on complexation and validated experimentally. It is shown that the chemical potential of an anion varies between melts as influenced by the different cations present in each melt. Hence, attempts to use a common electrochemical reference reaction for different salt mixtures are at best an approximation.