A spherical cellulose-based adsorbent (2-AMP resin) functionalized by 2-aminomethyl-pyridine was prepared via the radiation grafting technology. The adsorption behavior of the 2-AMP resin for Ag(I) recovery was assessed by batch and column experiments. The adsorption isotherm was best represented by Langmuir isotherm, and the adsorption capacity of the 2-AMP resin was 110.5 mg/g. The adsorption kinetics was found to follow the pseudo-second-order kinetic model. Moreover, the adsorbent presented good selectivity for Ag(I) from the coexisting ions [Ca(II), Mg(II), Ni(II), and Zn(II)] both in the batch and column experiments. The adsorption efficiency was unchanged even when the NaNO3 concentration was about 3000 fold higher than Ag(I). The interactions between the 2-AMP resin and Ag(I) were interpreted through XPS analysis, and the adsorption mechanism was proved to be a chelation interaction between aminomethyl-pyridine groups and Ag(I). It is demonstrated that the 2-AMP resin would have a splendid potential for the recovery of Ag(I).