The optimal geometries, mechanical and thermal properties, and electronic structures of the three low index (0 0 1), (1 1 0), (1 1 1) Ni/Ni3Al thin film were studied using first principle calculations. Simulated results indicated that Ni and Al atoms in gamma' phase preferred to place in the hollow site of Ni atoms in g phase. In hollow sitemodels, electronic states affected by interface localize within 2 atomic layers. While the top site model, electronic states localize within 3 atomic layers. It is also found that hollow site (1 1 0) interface has the best mechanical properties. Hollow site (0 0 1) interface is the most easily formed interface, which has the best thermodynamic properties. (C) 2008 Elsevier B. V. All rights reserved.