In this study, a new kind of thin 2D MOFs nano-sheets (MNS) was successfully prepared through complexation between 2-methylimidazole and Cu(II) by a one-step, and cost-effective route. The structural morphologies can be tuned by adjusting the ratio of MeOH/H2O The synthesized MNS (MNS-1, MNS-2, MNS-3 and MNS-4) were fully characterized and the results indicated that the synthesized MNS were freestanding and possess micro-sized lateral dimensions and nanoscale thickness of sub-25 nm. All the obtained MNS display great performance with the adsorption capacity hierarchy of MNS-2 (591.79 mg.g(-1)) > MNS-3 (409.49 mg.g(-1)) > MNS-4 (387.07 mg.g(-1)) > MNS-1 (384.84 mg.g(-1)) at pH (similar to) 6.0, and 298 K. The thermodynamic parameters indicated the exothermic and spontaneous nature of U(VI) immobilization. The U(VI) immobilization mechanism was achieved through the complexation between U(VI) and C-N(H) / - OH groups. This work supplies a facile and purposeful approach for developing 2D MOFs nano-sheets toward a highly efficient immobilization of U(VI), and it also promotes the preparation of structure-based design of nanomaterials for radionuclide-containing-medium pretreatment.