The cross-linking carboxymethyl starch was prepared using the cassava starch mechanically activated for 60 min by a ball-stirring mill. The static adsorption behavior and kinetics of the cross-linking carboxymethyl starch on Cr3+ were investigated. The adsorption mechanism was studied. The results showed that the cross-linking carboxymethyl starch could adsorb Cr3+ with 15.3 mg/g when the dosage of cross-linking carboxymethyl starch was 0.10 g, Cr3+ initial concentration was 0.06 mg/mL with pH of 3.3 and the adsorption time of 60 min. The adsorption was an intraparticle diffusion process. The adsorption process was adapted to Freundlich equation. The adsorption was comprehensive action of physical adsorption and chemical adsorption.