Hindered by the separation among radioactive elements, aluminum (Al), and rare earth elements (REEs), acid methods encounter persistent obstacles in reduction emission of ion-adsorption rare earth elements low-level radioactive residues (IREEs-LRR). This work reported a stepwise strategy for the reduction of emission and recovery of Al and uranium (U) from IREEs-LRR by alkaline and alkalescent media. As one of the main phases, Al(III)-containing compounds of IREEs-LRR were first converted into soluble NaAl(OH) 4 with NaOH solution at ordinary pressure. Na 2 U 2 O 7 and the adsorbed state U(VI), as detected by speciation, were then transformed into soluble uranyl carbonate in a Na 2 CO 3 -NaCit solution. The total removal yields of Al and U approached 97 and 94 wt %, respectively, engendering an 84 wt % loss weight of IREEs-LRR. Additionally, the REEs content in the residues increased from 0.88 to 3.6 wt %, while the specific activity of U decreased from 5.6 to 1.9 Bq/g. The mechanism was related to the NaOH-mediated dissociation of Al(III) polymeric complexes coupled with the enhanced dissolving capacity of uranium (U(VI)) complexes in alkalescent medium. This paper provides a novel strategy for reducing residual radioactivity, enriching REEs, and recovering valuable Al and U from IREEs-LRR.