The training dataset consists of measurements of 70 neat liquid densities (𝜌), 485 densities of binary mixtures (𝜌 𝑚𝑖𝑥 ), and 477 enthalpies of mixing of binary mixtures (Δ𝐻 𝑚𝑖𝑥 ). These measurements are selected at close-to-ambient conditions (99.9-101.4 kPa, 288.15-318.15 K), and are selected from molecules containing only hydrogen, carbon, nitrogen, oxygen, chlorine, and bromine. The measurements represent a diverse range of functional groups, chosen so that each included functional group includes at least 5 measurements. Long-chain alkanes and ethers were excluded due to difficulty packing simulation boxes and long correlation times in simulation, while 1,3-diketones were excluded due to their propensity for ketone-enol tautomerism. For physical properties of binary mixtures, we attempt to select 3 measurements at concentrations close to (𝑥 1 = 0.25, 𝑥 2 = 0.75), (𝑥 1 = 0.5, 𝑥 2 = 0.5), (𝑥 1 = 0.75, 𝑥 2 = 0.25), respectively. We enforced a minimum concentration of 𝑥 𝑖 = 0.05 for any component of a binary mixture, to avoid problems with sampling and convergence caused by a low absolute number of molecules of that component in a simulation box. Data in the ThermoML Archive includes expanded 95% CI uncertainty estimates provided by NIST, estimated either through uncertainty propagation or internal validation of methods/data consistency. While these uncertainty estimates are not directly used in the training process, they provide additional confidence in the data. This dataset is available at .