We report here on applying electric fields and dielectric media to achieve controlled alignment of single-crystal nickel silicide nanowires between two electrodes. Depending on the concentration of nanowire suspension and the distribution of electrical field, various configurations of nanowire interconnects, such as single, chained, and branched nanowires were aligned between the electrodes. Several alignment mechanisms, including the induced charge layer on the electrode surface, nanowire dipole-dipole interactions, and an enhanced local electrical field surrounding the aligned nanowires are proposed to explain these novel dielectrophoretic phenomena of one-dimensional nanostructures. This study demonstrates the promising potential of dielectrophoresis for constructing nanoscale interconnects using metallic nanowires as building blocks.