Eco-friendly dyeing by using supercritical carbon dioxide as a medium has already been investigated worldwide due to the advantages of dyeing without water and recyclability of dyes and carbon dioxide. In this article, dyeing mechanism of poly(m-phenylene isophthalamide) was investigated in supercritical carbon dioxide. The obtained results showed that the dye uptake of Disperse Red 60 increased moderately with the temperature raising at constant pressure and achieved dyeing equilibrium after 70 min. By adding the carrier, diffusion coefficients of Disperse Red 60 in the polymer increased significantly in supercritical carbon dioxide. The activation energy for diffusion of Disperse Red 60 with and without carrier was 1165.91 and 1050.66 kJ mol−1, respectively. Moreover, the distribution coefficient, the standard affinity, the standard enthalpy, and the standard entropy of dyeing were also determined in supercritical carbon dioxide. These fundamental data are of vital importance on the green dyeing production of poly(m-phenylene isophthalamide).