NdTbCo/Cr amorphous films with high perpendicular magnetic anisotropy were prepared onto glass substrates by rf magnetron sputtering. The effects of Nd substitution on the magnetic and magneto-optical properties of TbCo/Cr films were investigated. It was found that partial Tb substitution by Nd would increase the saturation magnetization and the Kerr rotation angle, change the temperature dependence of magneto-optical characteristics. These results can be explained by the ferrimagnetic structure of the rare earth-transition metal alloy. When the magnetic layer composition was (Nd0.265Tb0.735)31Co69, a saturation magnetization of 247 emu/cm3 and a coercivity of 3.8 kOe at room temperature could be obtained.