Superparamagnetic nanocomposite microparticles (NCMPs) modified with various layered double hydroxides (LDHs) (MgFe, MgAl and their Zr-doped equivalents) were investigated for phosphorus (P) removal. Screening of optimum composition was performed based on the P removal performance of NCMP@LDH particles as well as their magnetic separability in a flow-through column as a function of NCMP content (100-1000 mg) and stability as a function of LDH content (20-100%). The results showed that except for NCMP@MgFe-Zr, all the other particles exhibited a partial dissolution of LDH components at each of the examined LDH contents. However, NCMP@MgFe-Zr showed no dissolution up to a LDH content of 60% at all, whereas a partial dissolution occurred at a LDH content of 80 and 100%. Results of magnetic separability test revealed that the NCMP@MgFe-Zr composed of 500 mg magnetic particle (NCMP) and 60% LDH was separated from the solution with a separa-tion efficiency of 96.9%, while lower NCMP contents resulted in lower separation efficiencies. P removal effi-ciency and specific removal capacity of the NCMP@MgFe-Zr with the optimized composition was found to be 18.5% and 53.1 mg/g, respectively. The crystal structure, chemical composition, surface morphology, crystallite size and particle size distribution, functional groups and magnetic properties of the NCMP and NCMP@MgFe-Zr particles were confirmed by various characterization analysis. The observed results clearly demonstrates that the NCMP@MgFe-Zr with the optimized composition remained stable during the removal experiments and enabled the removal of P under the conditions of acidic pH and relatively high P concentration without LDH dissolution.