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A novel membrane capacitive deionization (MCDI) device, integrating both the advantages of carbon nanotubes and carbon nanofibers (CNTs–CNFs) composite film and ion-exchange membrane, was proposed with high removal efficiency, low energy consumption and low cost. The CNTs–CNFs film was synthesized by low pressure and low temperature thermal chemical vapor deposition. Several experiments were conducted to compare desalination performance of MCDI with capacitive deionization (CDI), showing that salt removal of the MCDI system was 49.2% higher than that of the CDI system. The electrosorption isotherms of MCDI and CDI show both of them follow Langmuir adsorption, indicating no change in adsorption behavior when ion-exchange membranes are introduced into CDI system. The better desalination performance of MCDI than that of CDI is due to the minimized ion desorption during …