The potential use of thorium (Th) and uranium (U) as nuclear fuels underscores the importance of developing materials for their sustainable recovery. The production of Th and U requires the separation of these elements from rare-earth elements (REEs) as they often coexist in various feedstocks. Equally crucial is efficiently isolating scandium (Sc) from REEs, considering its high-value status and pivotal role in advanced alloy technologies. This study introduces a new selective ligand-functionalized silica sorbent for extracting Sc, other REEs, Th, and U from solutions with varying pH and elemental compositions. The functionalized sorbent exhibits exceptional selectivity for Sc ions at pH 4 across solutions containing 3–20 elements. It also shows excellent selectivity for Th at pH 2 in 18- and 20-element solutions and substantial selectivity for U in 18- and 20-element solutions at pH 4. Additionally, it efficiently adsorbs neodymium (Nd), dysprosium (Dy), and lanthanum (La) in Sc-free solutions with a given preference for Nd. The ligand-functionalized sorbent successfully undergoes ten cycles of reuse which along with its enhanced recovery performance toward targeted elements highlights its industrial application potential.