Abstract: The first-principle method based on density-functional theory was used to investigate the geometries of the lowest-lying isomers of Au_n-2Ni₂ (n=3-7) clusters.Several low-lying isomers were determined, and many of them in electronic configurations had a high spin multiplicity.The stability trend of Ni-doped Au_n clusters was compared to that of pure Au_n clusters.The results show that the gold–nickel interaction is strong enough to improve the cluster stability, and indicate that the larger the Au_n cluster is, smaller the distortions by the two Ni atoms substitution are.It is observed that an odd-even alteration of the HOMO–LUMO gaps with the even numbered clusters is relatively more stable than the neighbouring odd-numbered ones.