Neodymium (Nd) and dysprosium (Dy) are two critical rare earth elements for fabricating NdFeB permanent magnets, which have crucial applications in modern technologies. The increasing global demand for Nd and Dy emphasizes new efficient processes for their recovery and purification, which are technologically challenging due to their close physical and chemical properties. Through systematic exploration, it was found that Lewatit VP OC 1026 resin impregnated with di-(2-ethylhexyl) phosphoric acid (D2EHPA) had a strong adsorption preference for Dy³⁺ over Nd³⁺, which is highly suitable for Dy-Nd separation from their mixed solutions under optimized conditions. The loaded resin could be eluted using dilute sulfuric solutions for recycling to the adsorption process. By employing a multistage adsorption-elution process analogous to distillation, efficient Dy-Nd separation and purification were realized from their mixed solution, with a prospective purity of 99.13% and recovery of 97.45% for Dy and a prospective purity over 99.96% and recovery of above 99.90% for Nd, despite the large concentration disparity between Dy and Nd where Nd concentration is over 26 times of that of Dy. This research demonstrates that efficient recovery and purification of metals from aqueous solutions can be achieved using selective resin adsorption processes analogous to distillation, despite large concentration differences of the metals in the solutions, which presents new alternative approaches.