In order to solve the problem of difficult recovery of metal-organic skeleton material UiO-66 in water and further improve the adsorption efficiency of UiO-66 to Cr(Ⅵ), molybdenum disulfide (MoS2) was doped to prepare UiO-66-NH2/MoS2. Then, the composite material was uniformly grown on polyurethane foam (PUF) by in-situ growth method to prepare the composite material UiO-66-NH2/MoS2@PUF. UiO-66-NH2/MoS2@PUF were characterized by XRD, SEM, TEM, TGA and BET. The results showed that UiO-66-NH2/MoS2 was uniformly loaded on the surface of PUF and the loading rate was up to 28%. The application experiment results showed that when pH was 4, the removal rate of Cr(Ⅵ) reached to 89%. After 5 cycles of adsorption, the removal rate of UiO-66-NH2/MoS2@PUF to Cr(Ⅵ) still was 83%, which indicated that UiO-66-NH2/MoS2@PUF had good recyclability. The concentration of Zr(Ⅳ) in the residual solution after Cr(Ⅵ) adsorption was analyzed. The concentration of Zr(Ⅳ) was 0.0785 mg/L, which indicated that the leakage of Zr(Ⅳ) during the adsorption process can be negligible and proved that UiO-66-NH2/MoS2@PUF had excellent chemical stability. The results showed that quasi-second-order kinetic model and Langmuir model can describe the adsorption process of UiO-66-NH2/MoS2@PUF to Cr(Ⅵ) well.