The thermal energy storage properties of a working fluid can be modified by the exothermic and endothermic adsorption and desorption of fluid molecules in the micro/nanoporous materials. In this study, thermogravimetric (TG) analysis experiments and molecular simulations (molecular dynamics, MD, and grand canonical Monte Carlo, GCMC) were employed to examine the thermal energy storage properties of the UIO-66 metal organic framework material, UIO-66/H2O nanofluids and pure water. Our results showed that the molecular simulation calculations were, in principle, consistent with the obtained experimental data. The thermal energy storage performance of UIO-66/H2O nanofluids was enhanced with the increase in the UIO-66 mass fraction. In addition, the differences between the simulation calculations and experimental results could be mainly ascribed to the different structures of UIO-66 and the evaporation of fluid samples. Furthermore, this work indicated that molecular simulations contributed to developing novel working pairs of metal organic heat carriers (MOHCs).