Nitriding surface hardening is commonly used on steel components for high wear, fatigue and corrosion applications. Case hardening results from white layer formation and coherent alloy nitride precipitates in the diffusion zone. This paper evaluates the microstructure development in the nitrided case and its effects on the hardness in both the white layer and the substrate for two industry nitriding materials, Nitralloy 135M and AISI 4140. Computational thermodynamic calculations were used to identify the type and amount of stable alloy nitrides precipitation and helped explain the differences in the white layer hardness, degree of porosity at the surface, and the hardening effect within the substrate. Some initial insights toward designing nitriding alloys are shown.