To better understand the imperfection influence on the ultrananocrystalline diamond (UNCD) properties under various loading conditions, a numerical study is performed to investigate the effect of vacancies on the mechanical responses of pure and nitrogen (N)-doped UNCD films under tensile and shear loading paths at elevated temperatures. A simple procedure is developed by combining kinetic Monte Carlo with molecular dynamics (MD) methods to form a polycrystalline UNCD block. Different numbers of vacancies are introduced by randomly removing carbon atoms from the resulting UNCD blocks. The responses of the simulated pure and N-doped UNCD blocks with different numbers of vacancies are then investigated by applying displacement–controlled loading under different temperatures in the MD simulations. The simulation results presented in this paper provide a better understanding of the imperfection effect on the mechanical responses of pure and N-doped UNCD films as compared with the grain boundary effect.