This study presents a new, revolutionary, and easy method of separating Gd (III). For this purpose, a cellulose acetate membrane surface was modified in three steps, as follows: firstly, with aminopropyl triethoxysylene; then with glutaraldehyde; and at the end, by immobilization of crown ethers. The obtained membranes were characterized by Fourier transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS), through which the synthesis of membranes with Gd (III) separation properties is demonstrated. In addition, for the Gd (III) separating process, a gadolinium nitrate solution, with applications of moderator poison in nuclear reactors, was used. The membranes retention performance has been demonstrated by inductively coupled plasma mass spectrometry (ICP-MS), showing a separation efficiency of up to 91%, compared with the initial feed solution.