The macroporous thiocarbohydrazide crosslinked chitosan-poly(vinyl alcohol) framework (TCPF), prepared via the condensation reaction of thiocarbohydrazide and the oxidized products of chitosan (OCS) and poly(vinyl alcohol) (OPVA) is reported with selective and efficient adsorption of Cu(II), Pb(II), and Hg(II). The adsorption of Cu(II), Pb(II), and Hg(II) onto TCPF was studied through batch adsorption experiments, and the adsorption data were analyzed by using various models. The Langmuir model fits best with the experimental values which yields adsorption capacities of 47.16 mg g −1 , 47.39 mg g −1 , and 52.63 mg g −1 for Cu(II), Pb(II), and Hg(II), respectively. The calculated thermodynamic parameters ΔG o , ΔS o , and ΔH o suggest that the adsorption of Cu(II), Pb(II), and Hg(II) is thermodynamically favorable and thus a spontaneous process which follows pseudo-second-order kinetics. The plot of qt versus t 1/2 suggests that intraparticle diffusion is not only the ratecontrolling step but also the positive value of the intercept in Pb(II) and Hg(II) plots. This indicates that several steps are operational in the adsorption mechanism. Furthermore, the excellent recycle performances also were achieved with desorption and regeneration efficiencies close to 97−99%, permitting the recovery of both metal ions and TCPF. Finally, the complete soil degradability which can be attained in approximately 90 days makes the whole process environmentally friendly and economically feasible.