The radioactive pollution of uranium-containing effluent seriously harms environmental safety and human health. Herein, the honeycomb-like ion-imprinted chitosan/ZSM-5 (ICZ) composite foams were prepared and used for the selective sorption of U(VI). The results suggest that ICZ-2 is the best among various ICZ foams with different raw material ratios, owing to its well-developed honeycomb-like structure as well as the presence of abundant functional groups. Compared to the non-imprinted sorbent, the ion-imprinted sorbent ICZ-2 presents higher sorption and better selectivity since it could smartly recognize the target ions. The sorption isotherms could be described by Langmuir model, suggesting homogeneous monolayer sorption with the maximum sorption capacity of 280.09 mg/g. The sorption kinetics could be fitted by the pseudo-second order model, indicating chemisorption as the rate-controlling step. The main sorption mechanism is related to U(VI) coordination by the functional groups of ICZ-2. The ICZ-2 presents a high sorption capacity, fast kinetic rate, and good selectivity for U(VI), therefore it has potential applications for the treatment of U(VI) –containing wastewater.