In this work, ultrasonication-assisted deposition technology was used to prepare the composite poly(vinylidene fluoride) (PVDF)/graphene oxide (GO) membrane with regarding to organic dyes removal. The electrospun PVDF fibrous membrane, which was first obtained through electrospinning technology, was immersed into the GO aqueous solution, and then the mixture was ultrasonically treated at power of 100 W for different time. Microstructure characterizations and hydrophilicity measurements confirmed that many GO platelets were incorporated into the PVDF membrane. The adsorption ability toward methylene blue (MB) by the composite PVDF/GO membrane was then systematically investigated. The results showed that the ultrasonication time and the concentration of GO in the aqueous solution determined the content of GO in the composite membrane, which also determined the adsorption capacity of the composite membrane. Studies on adsorption kinetics and adsorption isotherms showed that the adsorption behavior of the composite PVDF/GO membrane could be well described by the pseudo second-order model, and the maximum adsorption capacity of MB was 621.1 mg g(-1). Furthermore, the composite PVDF/GO membrane exhibited excellent regeneration ability. This work demonstrates that the composite PVDF/GO membrane may be a promising adsorbent to remove organic dyes from wastewater.