Many efforts have been made to enhance the yield strength of high-Mn austenitic steel, but the methods, including grain refinement through severe plastic deformation and hierarchical microstructure design, have certain limitations in industrial application, especially the thick plate, and the cryogenic toughness is also decreased. In the present work, two high-Mn austenitic steels with 0.6/0.8 wt% carbon additions were fabricated to strengthen the high-Mn austenitic steel, and the effects of carbon on microstructural evolution and the resultant strength, cryogenic toughness (−196 °C) were revealed. The results show that the yield strength of 0.8C steel can be dramatically improved by 121 MPa compared to 0.6C steel, but at the same time, the two steels exhibit excellent and similar cryogenic impact energies, both above 120 J. The strengthening modes of 0.6C steel contain four kinds of grain refinement, solid-solution, dislocation and precipitation, so does the 0.8C steel. The substantially increased yield strength of 0.8C steel is derived from solid-solution and precipitation strengthening. Under impact loading at −196 °C, the main deformation modes of 0.6C steel are dislocation glide and cross twinning, resulting in ductile dimpled fracture and high cryogenic toughness. As for 0.8C steel, the difference with 0.6C steel is that there exist fewer deformed grains in as-hot rolled microstructures due to the facilitation effect of high carbon addition on recrystallization and recovery, which promotes dislocation glide and twinning formation. Besides, the fine nanoscale VC carbides are also conductive to maintaining the high toughness while improving strength. Hence, the high cryogenic toughness can be retained in the 0.8C steel. The yield strength and cryogenic toughness of 0.8C steel reach 624 MPa and 123 J, respectively, greatly superior to the reported high-Mn austenitic steels.