A novel magnetic calcium silicate hydrate composite (Fe3O4@CSH) was proposed for phosphorus (P) removal and recovery from a synthetic phosphate solution, facilitated by a magnetic separation technique. The Fe3O4@CSH material was characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), powder Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), zeta-potential and magnetic curves. The chemical composition and structure of Fe3O4@CSH and the successful surface loading of hydroxyl functional groups were confirmed. Phosphate adsorption kinetics, isotherm, and thermodynamic experiments showed that adsorption reaches equilibrium at 24 h, with a maximum adsorption capacity of 55.84 mg P/g under optimized experimental conditions. Adsorption kinetics fitted well to the pseudo second-order model, and equilibrium data fit the Freundlich isotherm model. Thermodynamic analysis provided a positive value for ΔH° (129.84 KJ/mol) and confirmed that phosphate adsorption on these materials is endothermic. The P-laden Fe3O4@CSH materials could be rapidly separated from aqueous solution by a magnetic separation technique within 1 min. A removal rate of more than 60% was still obtained after eight adsorption/desorption cycles, demonstrating the excellent reusability of the particles. The results demonstrated that the Fe3O4@CSH materials had high P-adsorption efficiency and were reusable.