High Mn steels demonstrate an exceptional combination of high strength and large ductility as a result of their high strain-hardening rate during deformation. The microstructure evolution and strain-hardening behavior of Fe18Mn0.6C1.5Al TWIP steel in uniaxial tension were examined. The purpose of this study was to determine the contribution of all the relevant deformation mechanisms—slip, twinning, and dynamic strain aging. Constitutive modeling was carried out based on the Kubin–Estrin model, in which the densities of mobile and forest dislocations are coupled to account for the interaction between the two dislocation populations during straining. These coupled dislocation densities were used to simulate the contribution of dynamic strain aging to the flow stress. The model was modified to include the effect of twinning. To ascertain the validity of the model, the microstructural evolution was characterized in detail by means of transmission electron microscopy and electron back-scatter diffraction.