Gd2O3 has been considered as a kind of good host material for photoluminescence. The method of laser ablation in liquid (LAL) is increasingly used for the preparation of Gd2O3 because it is green and usually simple. In this work, monoclinic Gd2O3:Tb3+/Eu3+ nano-phosphors were successfully synthesized by LAL method. The morphology, structure, and optical properties of the nano-phosphors were discussed. The color of fluorescence of Gd2O3:Tb3+/Eu3+ nano-phosphors were successfully turned by controlling the content of Tb3+ and Eu3+ . The results show that the synthesized Gd2O3:Tb3+/Eu3+ nano-phosphors are potential to be applied to display, lighting, biological imaging or other fields.