Covalent organic frameworks (COFs) with regular and tailorable pore channels are promising for constructing advanced adsorbents for the recovery of rare earth ions. However, it remains a challenge to construct composite adsorbents comprising COFs with well-defined morphologies. This study describes a composite bead composed of a polyacrylonitrile matrix and a negatively charged COF, TpPa-SO3Na, possessing a strand-like morphology for the extraction of Nd3+ from aqueous solutions. Porous and crystalline TpPa-SO3Na nanostrands were synthesized under hydrothermal conditions and exhibited a high adsorption capacity (107.1 mg g–1), fast kinetics, and good selectivity during Nd3+ adsorption. TpPa-SO3Na nanostrands were further processed into composite beads with a high loading amount of 50%, and the resulting beads effectively maintained the original microstructures and properties of the nanostrands. Importantly, the composite beads can be used in a dynamic process and show excellent recovery efficiency under low or high Nd3+ concentrations as well as good operational stability. This work not only demonstrates an evident strategy for preparing composite beads by leveraging a polymer matrix and COF nanostrands but also highlights their great potential in the extraction of sparse precious metal resources, including but not limited to rare earth ions.