A renewable metal–organic-frameworks (MOFs)-polylactic acid (PLA) film was designed and prepared in order to remove malachite green (MG) in waste water. The PLA frame was prepared by three-dimensional (3D) printing technology, followed by in situ step-by-step growth of Cu-MOFs on its surface. The printed PLA skeleton and the prepared Cu-MOFs/PLA films were characterized by scanning electron microscopy and X-ray powder diffraction. The adsorption capacity of Cu-MOFs/PLA films towards MG was then investigated. Results showed that more than 90% removal efficiency was observed in adsorbing MG of different concentrations for 10 min. Practical applications of Cu-MOFs/PLA films for removal of MG in waste-water samples were then demonstrated. The used Cu-MOFs/PLA films were found to be recyclable over more than five times after simple washing with acetone. In addition, it was noted that the PLA skeleton could be recovered for the further growth of Cu-MOFs on its surface. The successful development of this technique provides a new strategy for the design of renewable materials for the adsorption of organic dyes in waste water, which holds enormous potential for broad applications in waste-water treatment.