Taking ZrN as a model catalyst for NRR, we have optimized the MOCVD route to grow oriented crystalline ZrN layers with facetted growth along the (100) plane on Si and GC substrates. This is the first case study where CVD grown ZrN material system has been investigated from a point of view using it for NRR. The specific choice of the Zr precursor comprising of a preformed Zr-N bond enables the controlled growth of ZrN. This was proved experimentally and theoretically where the SSP decomposition reaction pathway towards nitride thin films was elucidated. Compositional analysis revealed slightly nitrogenrich films with a certain amount of oxygen incorporation. XPS sputtering study indicates post deposition oxidation, predominantly on the surface which is also demonstrated by an aiMD calculation of a model ZrN(100) surface reacting with O atoms under ambient conditions yielding a surface termination of ZrO/ZrN. SEM reveals a high surface area of the films and cross-sectional BF-TEM illustrated a columnar growth on both substrates. Furthermore, STEM-EDS and SAED reveal an even distribution of Zr and N throughout the film as well as crystalline rock salt ZrN, respectively. Band gap energies were found to be thickness dependent which increase with a decrease in thickness. This suggests a self-limiting surface oxidation of the ZrN films under ambient conditions since a thinner film has a relatively larger ZrOxNy region. Electrochemical CV experiments of the ZrN films on GC in Ar-and N2-saturated electrolyte