Recycled Nd and Dy from the end-of-life NdFeB permanent magnet is an important supplement for the increasing demand of rare-earth elements. Thus, there is an urgent need to develop an environmentally friendly recycling method. Amorphous zirconium phosphate exhibits selective separation properties towards the ternary Co-Nd-Dy system, however, its powdery form limits development of scaled-up applications. We present an efficient amorphous ZrP/Polyacrylonitrile (am-ZrP/PAN) composite ion exchanger for uptake and separation of Nd, Dy and Co. The am-ZrP/PAN composite was synthesized and its structural, morphologic and acidic properties were investigated by various methods. X-ray tomography revealed rather evenly distributed am-ZrP in the PAN polymer matrix. The selectivity and ion-exchange kinetics of the am-ZrP/PAN composite were determined in relation to the individual elements. Due to dimethylformide (DMF) intercalation into the interlayer of ZrP, the uptake of Co, Nd and Dy increased 50% compared with that of the pristine am-ZrP. Column separation of Co, Nd and Dy from the Co-Nd-Dy ternary system was assessed by varying the feed concentration, loading degree, temperature, running speed and elution agent (HNO3) concentration. Finally, gradient elution was employed for Co, Nd and Dy separation from a simulated ternary leachate. Fractions with 87.9% pure Co, 96.4% pure Nd and 40% pure Dy were collected through a single-column operation.