A study is conducted to simulate the simultaneous deposition of Ni and Al atoms on Ni(0 0 1) substrate by molecular dynamics. The effects of deposition conditions and annealing on microstructure and morphology of the NiAl films are investigated. The empirical embedded-atom method is applied to calculate the atomic interactions between Ni and Al atoms. The simulative results indicate that increasing incident energy can roughen the surface of un-annealed films in 15 eV, enhance intermixing between film and substrate, strengthen the destruction to the perfect crystal structure of substrate from incident atoms, and increase the content of vacancies and voids in 10 eV. While incident angles have little influence on surface roughness (in 30 degrees), intermixing, and destruction to the substrate, only density changes with incident angle by direct proportion. The substrate temperature almost has the same but weaker effect with incident energy on these properties, except for the density. After annealed, the films become smoother and more homogeneous, ordered and compact. (C) 2015 Elsevier B.V. All rights reserved.