Layered graphene oxide film, LGOF, was prepared via the layer-by-layer electro-assembly, LBLEA, method. The LGOF formed by applying the voltage at 4 kV and the electrostatic forces, EF, in reduction state showed transparent aspect as the same as the 0 V formed sample that was obviously unlike the 4 kV-EF-enhancement formed sample in opaque. FESEM images showed the morphology of LGOF surface was controlled by voltage variety and EF-control. AFM images revealed that the LGOF surface formed by EF-reduction was in nano-needle structure and by EF-enhancement was in nano-heap structure. ATR-FTIR and XRD analyses indicated that the LGOF formation process would led the GO reduced to RGO, when the EF weakly can keep the hydrophilic functional groups on LGOF surface while the EF strongly unable. Water contact angles on 0 V formed LGOF surface was at about 36 degrees and reduced with the voltage increase, especially by controlling the EF because on 4 kV-EF-enhancement formed sample surface was at about 12 degrees and on 4 kV-EF-reduction formed sample surface was at about 5 degrees approaching the superhydrophilic. A comparison found that the superhydrophilic LGOF has enhanced conductivity and dye adsorption than that of the other samples prepared also by the LBLEA method. (C) 2018 Elsevier B.V. All rights reserved.