We have fabricated Ni3Al and NiAl thin films on different substrates by the pulsed laser deposition (PLD) technique. A high energy nanosecond laser beam was directed onto Ni–Al (NiAl, Ni3Al) targets, and the evaporated material was deposited onto substrates placed parallel to the target. The substrate temperature was varied between 300 and 400 °C, and the substrate-target distance was maintained at approximately 5 cm. The films were analyzed using scanning electron microscopy, transmission electron microscopy, x-ray diffraction, and Rutherford backscattering spectrometry. At energy densities slightly above the evaporation threshold, a slight enrichment of Al was observed, while at higher energy densities the film stoichiometry was close (<5%) to the target composition. Barring a few particles, the surface of the films exhibited a smooth morphology. X-ray and TEM results corroborated the formation of Ni3Al and NiAl films from similar target compositions. These films were characterized by small randomly oriented grains with grain size varying between 200 and 400 Å.