In this study, phosphorus removal from aqueous solution was investigated using chitosan/Ca-organically modified montmorillonite (chitosan/Ca-OMMT) beads in batch and fixed-bed column systems. The XPS spectra confirmed that the calcium ions on the surface of the beads play a dominant role in capturing phosphate ions through surface complexation. The batch adsorption experimental data were fitted with pseudo-second-order kinetics and the Langmuir isotherm. The maximum adsorption capacity of the chitosan/Ca-OMMT beads was found to be 76.15 mg/g at an initial phosphate concentration of 100 mg/L at 25 degrees C. High phosphate uptake is achieved over the wide pH range 3-11, as well as in the presence of competing anions such as Cl-, NO3-, SO42-, and HCO3-. Furthermore, the chitosan/Ca-OMMT beads can be easily regenerated using 0.1 mol/L NaOH as a desorption agent with more than 83.97% adsorption capacity remaining after five adsorption/desorption cycles. The Thomas, Yoon-Nelson, and Adams-Bohart models were applied to the experimental data to predict the breakthrough curves using non-linear regression; the Yoon-Nelson model showing the best agreement with the breakthrough curves. These findings demonstrate that chitosan/Ca-OMMT beads can be used as a cost-effective and environment-friendly adsorbent for the removal of phosphate from wastewater.