Here, we calculated a large number of infinite dilution activity coefficients and compared with experimental values extracted automatically from NIST's ThermoML database. We used relatively standard (if computationally demanding), easily-automated approaches for calculation of solvation free energies, and performed the calculations in a high-throughput manner on OpenEye's Orion cloud computing platform. This allowed the calculations to run in a highly parallel and relatively efficient manner and complete on an overnight timeframe. Interestingly, agreement between calculated and experimental values is actually quite good, and these calculations are also able to highlight clear systematic issues for particular functional groups or types of solutes/solvents, suggesting promising areas for investigation of possible force field deficiencies. The fact that infinite dilution activity coefficients can also be measured in a relatively straightforward manner means these will likely serve as a valuable source of data for future tests of computational methods.