In this study, a new method for predicting carbon and nitrogen contents of a carbonitrided surface using computational thermodynamics with Thermo-Calc was developed. The nitrogen content of alloyed steel, which is in equilibrium between the steel surface and the atmosphere, was predicted using the nitriding potentials and Thermo-Calc, and the experimental and calculated results were compared using pure iron. For lower nitrogen levels, the accuracy of prediction was sufficient. However, for higher nitrogen levels, the experimental nitrogen content was lower than the calculated value, which was attributed to pore formation. Through a comparison of the described method with the conventional one, it was confirmed that our novel prediction method exhibits sufficient accuracy to predict the nitrogen content following carbonitriding.