The nanomechanical properties of NbN/Nb deposited by pulsed laser deposition (PLD) were investigated as a function of the film/substrate crystal structure. In addition to the beta-Nb2N phase, the X-ray diffraction shows peaks correspond to delta-NbN cubic and delta '-NbN hexagonal phases. Several samples were tested of varied crystal structure between dominant cubic to dominant hexagonal. X-ray diffraction analysis, scanning electron microscopy, atomic force microscopy were employed to characterize their phases, microstructure, and surface morphology. Nanoindentation was used to investigate the nanomechanical properties of the films. A Nanoindenter XP equipped with a DCM II head was used in conjunction with the continuous stiffness method (CSM) in depth and load control modes to evaluate the hardness and modulus of the NbN thin films as a function of the crystal structure. The results show that there are clear effects of the crystal structure on the elastic modulus and hardness of the PLD-grown NbN films.