A new type of thiourea cross-linked chitosan with Fe(III) as template (TCCTS template) was synthesized. The adsorption of Fe(II) and Fe(III) on this TCCTS template was studied. The factors affecting adsorption such as pH and contact time were considered. The results showed that the optimum pH value for adsorption was pH = 5.0 and the adsorption equilibrium time was about 60 min. The adsorption isotherms and kinetics were investigated, and the equilibrium data agreed very well with the Langmuir model and the pseudo second-order model could describe adsorption process better than the pseudo first-order model. Results also showed that TCCTS template was a favourable adsorbent for Fe(II) and Fe(III) in aqueous solution.