The influence of nanosecond laser impulse irradiation on the magneto-optical properties of multilayer film nanostructures Bi SiC TbFe SiC, SiC TbFe SiC, SiC Tb Au Fe SiC, and phthalocyanine dye-bismuth-phthalocyanine dye was investigated. It was shown that this irradiation causes the injection of spin-polarized electrons from magnetic into nonmagnetic layers of the multilayer films. Nonequilibrium magnetization arising in nonmagnetic layers leads to the change of magneto-optical characteristics. The voltage induced by laser irradiation can also produce a directed drift of Bi ions toward the laser beam action.