Two novel chitosan (CS) adsorbents were prepared in powder form, after modification with the grafting of itaconic acid (CS-g-IA) and cross-linking with either glutaraldehyde (CS-g-IA(G)) or epichlorohydrin (CS-g-IA-(E)). Their adsorption properties were evaluated in batch experiments for Cd(II) or Pb(II) uptake. Characterization techniques were applied to the prepared adsorbents as swelling experiments, TGA, SEM, XRD, and FTIR. Adsorption mechanisms were suggested for different pH conditions. Various adsorption parameters were determined as the effect of pH, contact time, and temperature. The maximum adsorption capacities for Cd(II) uptake were 405 and 331 mg/g for CS-g-IA(G) and CS-g-IA(E), respectively, revealing the capacity enhancement after grafting (124 and 92 mg/g were the respective values before grafting, respectively). A similar grafting effect was observed for Pb(II) uptake, proving its adsorption effectiveness on the CS backbone. The reuse of adsorbents was tested with 20 adsorption-desorption cycles.