Graphene oxide (GO) based membranes are widely adopted in molecular separation based on size exclusion effect by stacked GO sheets. Both high flux and efficient rejection of GO-based membranes for long-term operation are highly expected for practical applications. Here, an attapulgite (ATP) nanofibers/ GO composite (ATP/GO) membrane is assembled by filtration of mixed aqueous colloidal suspensions of ATP and GO. Due to the modification of interlayer distance and surface property of GO membrane by ATP, the ATP/GO membrane demonstrates excellent separation performance, with a high water flux of 221.16 Lm hbar, 7.7 times higher than that of pure GO membrane. Meanwhile, the rejection of ATP/GO is also slightly improved comparing with that of GO membrane. It is also found that increasing the thickness of the membrane is effective to enhance rejection percentage. The ATP/GO membranes reported here show high efficiency for molecular separation, which demonstrates potential applications in water purification and environmental protection.