The synthesis of dimethyl toluene-2,4-dicarbamate from 2,4-toluene diamine and dimethyl carbonate is a complex reaction system. First, the reaction enthalpies, the Gibbs function changes, and the equilibrium constants of the reactions were calculated by several methods of group contribution. Secondly, the kinetics of the synthesis reaction over a zinc acetate catalyst was investigated in a batch autoclave. The kinetic model equations were established by parameter estimation based oil experimental data, and the model met the requirements of the statistical test. The calculated results based oil the model agreed well with the experimental data. According to the results of both thermodynamic calculation and kinetic analysis, the influence of some technological parameters, such as content of methanol in the feed and reaction temperature, oil the synthesis reaction was discussed.