Knowledge of the thermophysical properties of CO2-hydrocarbon mixtures over extended ranges of temperature and pressure is crucial in the design and operation of many carbon capture and utilization processes. In this paper, we report phase behavior, saturated-phase densities, and compressed-liquid densities of CO2 + methylbenzene at temperatures between 283 K and 473 K and at pressures up to 65 MPa over the full composition range. The saturated-phase densities were correlated by a recently developed empirical equation with an absolute average relative deviation (ΔAARD) of ∼0.5%. The compressed-fluid densities were also correlated using an empirical equation with an ΔAARD value of 0.3%. The new data have been compared with the predictions of two equations of state: the predictive Peng–Robinson (PPR-78) equation of state and the SAFT-γ Mie equation of state. In both of these models, binary parameters are estimated using functional group contributions. Both models provided satisfactory representation of the vapor–liquid equilibrium and saturated-phase-density data, but the accuracy decreased in the prediction of the compressed-liquid densities where the ΔAARD was ∼2%. The isothermal compressibility and isobaric expansivity are also reported here and were predicted better with SAFT-γ Mie than with PPR-78. Overall, the comparisons showed that SAFT-γ Mie performs somewhat better than PPR-78, but the results suggest that further refinement of the SAFT-γ Mie parameter table are required.