Advancements in membrane separation techniques will expand the applications and requirements for highly specialized, inventive, efficient, and resistant separation materials. The selective separation of rare earth elements (REEs) is one of the expanding applications of membrane-based techniques, as their use is becoming more widespread. Membrane techniques are becoming increasingly desired as environmentally friendly, straightforward methods for treating wastewater and separating metals. For the separation of REEs, an innovative impregnated mixed-matrix membrane (IMMM) technique was developed in this study. It provides a selective, efficient, and reusable method that is suitable for industrial applications. Terbium was selectively adsorbed from other REEs using organophosphorus IMMM with a loading capacity of 113.2 mg/g in 3 h and was reused three times without destroying the initial membrane. Solvent impregnation is thought to offer specific chelation sites that are selective for terbium separation.