This study show s that calcium silicate/aluminate-based materials can be carbonated to produce sorbents for metal removal. The material chosen for investigation, cement clinker, w as accelerated carbonated, and its structural properties w ere investigated using X-ray diffraction (XRD), scanning electron microscopy, thermal gravimetric and differential thermal analysis, nuclear magnetic resonance spectroscopy, and nitrogen gas adsorption techniques. The principal carbonation reactions involved the transformation of dicalcium silicate, tricalcium silicate, and tricalcium aluminate into a Ca/Al-modified amorphous silica and calcium carbonate. It w as found that carbonated cement had high acid buffering capacity, and maintained its structural integrity w ithin a w ide pH range. The uptake of Pb(II), Cd-(II), Zn(II), Ni(II), Cr(III), Sr(II), M o(VI), Cs(I), Co(II), and Cu-(II) from concentrated (1000 mg L -1 ) single-metal solutions varied from 35 to 170 mg g -1 of the carbonate cement. The removal of metals w as hardly effected by the initial solution pH due to the buffering capability of the carbonated material. The kinetics of Pb, Cd, Cr, Sr, Cs, and Co removal follow ed a pseudo-second-order kinetic model, w hereas the equilibrium batch data for Cu fitted the pseudofirst-order rate equation. PHREEQC simulation supported by XRD analysis suggested the formation of metal carbonates and silicates, calcium molybdate, and chromium (hydro)-oxide. Cesium w as likely to be adsorbed by Ca/Al-modified amorphous silica.