The chitosan/poly(acrylic acid) (CS/PAA) hydrogel was synthesized in aqueous solution using glow-discharge electrolysis plasma (GDEP) technique, in which chitosan and acrylic acid were used as materials, N,N'-methylenebisacrylamide (MBA) as a crosslinking agent. The structure of CS/PAA hydrogel was characterized by FT-IR, XRD and SEM. The effects of the solution pH, contacted time and initial metal concentration of Cu2 and Cd2 on the adsorption were investigated systematically. Moveover, the reusability of hydrogel was studied as well. The results showed that the acrylic acid has been successfully grafted into the chitosan backbone. The hydorgel exhibits a three-dimensional network structure with a large number of pores on the surface. The adsorption of hydrogel for Cu2 and Cd2 is agreed well with the pseudo-second-order kinetic model and the Langmuir isotherm model at room temperature. The maximum adsorption capacities of Cu2 and Cd2 obtained by Langmuir model are 161.8 and 327.9 mg/g, respectively. CS/PAA hydrogel displays excellent reusability using EDTA-4Na as eluent.