amines with oxygen-containing groups on GO. [17] Gao et al. manufactured GO paper by air drying and then exposing it in glutaraldehyde vapors to realize cross-linking, by which the mechanical properties of the resulting paper were largely improved. [18] Fang et al. covalently grafted polystyrene chains onto the surface of GO sheets and thereby increased the tensile strength and Young's modulus. [19] These prior studies proved that GO nanosheets could be grafted with appropriate molecules and polymers to introduce new functional groups and make GO more flexible and versatile in applications.GO has been extensively applied in transparent conductors, optoelectronics, and composite materials. [20][21][22][23] Recently, GO nanosheets have attracted interest in constructing membranes and the relevant applications. [24][25][26][27] Generally, composite membranes produced from porous materials, such as zeolite and carbon molecular sieves show excellent performance on separation, gas storage, and electrochemistry, [28][29][30][31][32][33][34] however, theses membranes still have some intractable problems such as brittleness, poor thermal stability, and weak mechanical strength. Compared with these materials, GO is believed to be one of the most promising separation membrane materials. GO membranes can be produced by vacuum filtration or layer-by-layer assembly, and both methods are environmentally friendly. [35][36][37][38][39][40][41][42] In the process of filtration, the GO or the modified GO nanosheets stack tightly, forming an ordered laminate structure to act as the separation layer of membrane. The GO membranes can be used in many fields like dye removal, desalination, and pervaporation; and the structure of GO layer has great effects on the performance of membrane. [43][44][45][46] In this work, we report a strategy to adjust the microstructure of GO nanosheets and the size of nanochannels by grafting polydopamine (PDA) on GO, by which to construct composite membranes via simple vacuum filtration. The degree of polymerization can be well controlled by reaction time. Through this method, the size of nanochannels formed by two GO sheets could be adjusted with different PDA loading. Thereby, the separation performance of the as-obtained membranes can be controlled accordingly. The membranes with controllable interlayer space are promising for diverse applications.Graphene oxide (GO) is a unique 2D material that can form nanochannels between adjacent nanosheets, and has attracted concentrated interests in the field of molecule sieving. However, the size of the nanochannels is fixed and hard to change, which is undesirable when using GO-based membranes for separation. Herein, a strategy for controllable adjusting the microstructure of GO nanosheets and size of nanochannels by grafting polydopamine (PDA) on GO is reported. A series of PDA-g-GO composite membranes with different PDA loading are successfully fabricated by simple vacuum filtration. The composite membranes are used to separate 70 wt% ethanol-H 2 O mixture an...