This study on thermodynamic property of NH -CO -H O system provided the basic data for ammonia carbonation. Simulations on vapor-liquid equilibrium (VLE) of ammonia carbonation with different physical properties were discussed in NH -H O and NH -CO -H O systems, respectively. The results indicated that at low temperature (303.15 K–363.15 K) and pressure (0.1–0.4 MPa), the PR (Peng-Robinson) equation was suitable for the description of the thermodynamic state in NH -H O system. NRTL (Non-Random-Two-Liquid) series models were selected for NH -CO -H O mixed electrolyte solution system. VLE data regression results showed that NRTL series models were suitable for describing thermodynamic properties of NH -CO -H O system, because average relative error fitting with each model was about 1%. As an asymmetric electrolytes model in NRTL model, E–NRTLRK (Electrolyte NRTL Redlich Kwong) could most accurately fit VLE data of NH -CO -H O system, with fitting error less than 1%. In the extent temperature range of 273.15 K–363.15 K, the prediction of product component using E-NRTLRK model for ammonia carbonation agreed well with the data reported in literature.