The importance of rare-earth elements (REEs) in the global economy is rapidly growing, since they are essential to many advanced technologies. Therefore, the development of more performant separation procedures for REEs has become necessary. In the present study, we used silica hybrid materials (SHMs), which were synthesized by an all-in-one approach that allows the direct incorporation of desired functional groups, as sorbent material. Promising results were obtained for the extraction capacities of diglycolamide-functionalized materials. Under the tested conditions, they showed high efficiency (Nd uptake capacity of about 25 mg per g of material) and high selectivity toward REEs from a simulated NdFeB magnet leachate. For these materials, Nd recovery after extraction was achieved with an efficiency of 80% by contacting the loaded material with distilled water at moderate pH (6.5).