Owing to their unique physicochemical features, ionic liquids (ILs) are extensively utilized to dissolve cellulose for the preparation of regenerated cellulose fibers (RCFs) in the textile industry. However, Cu2+ is introduced during the cellulose dissolution process and gradually accumulates, seriously affecting the RCF performance and IL recovery. Herein, to achieve an efficient and selective adsorption of Cu2+ from ILs aqueous solutions, a facile and green method based on the in situ growth of zeolitic imidazolate framework-67 in wood hydrogels (ZIF-67@WH) is presented. The morphology, functional groups, crystallinity, thermal stability, and pore structure of the resulting ZIF-67@WH were investigated using various characterization techniques, and the adsorption selectivity, adsorption thermodynamics, adsorption kinetics, and recoverability were examined in depth by performing batch experiments. The ZIF-67@WH exhibits high adsorption selectivity for Cu2+ and ILs with adsorption ratios of 92.8 % and 2.2 %, respectively. The selective adsorption mechanism was elucidated by means of FT-IR, XPS, DFT, and MD. As the key for the selective adsorption, the N site in ZIF-67 dramatically promotes the coordination with Cu2+, while the adsorption for ILs mainly occurs via hydrogen bonding and van der Waals interactions with adsorption energies of –80.61 and –35.33 kcal/mol, respectively. The results demonstrate that this approach constitutes a feasible technique for the efficient separation of Cu2+ and ILs in the textile industry.