The Mexican enhanced genetic algorithm has been used to study the structural and energetic properties of Pd, Ni, and Ni−Pd nanocluster structures with 3−10 atoms. Density functional theory (DFT) calculations have been performed to investigate the structural behavior, spin magnetic moment, and stability as a function of cluster size and composition. Various stability criteria (for example, binding energies, second differences in energy, and mixing/excess energies) have been used to evaluate the energetics, structure, and tendency to segregation in subnanometer Ni−Pd clusters. The ability of the approach in searching for global minima (i.e., the lowest-energy isomers) has been assessed using a systematic homotop search of monosubstituted clusters and the preferred doping sites.