This paper investigates the relationship between the physical properties of NbN thin films and a series of different substrates/buffer layers used for the thin film growth. Substrates, including 4H-SiC, AlN/Si, AlN/sapphire, and annealed AlN/sapphire, were selected for NbN film deposition via DC magnetron sputtering. Post-deposition annealing was also employed to study its impact on the films’ quality. Comprehensive characterizations were performed on NbN films, focusing on superconducting critical temperature (T_C), transition width (ΔT_C), crystalline quality, and surface roughness. The results demonstrate that the annealed NbN films grown on 4H-SiC substrates with the highest crystalline quality exhibit optimal crystalline quality, achieving a T_C of 16.3 K. Experimental results reveal intrinsic correlations between the critical properties of NbN superconducting thin films and substrate structural characteristics; the impact of post-growth annealing on the T_C is also studied.