New hierarchical bioinspired nanocomposite materials of poly(vinyl alcohol)/poly(acrylic acid)/carboxylate graphene oxide nanosheet@polydopamine (PVA/PAA/GO-COOH@PDA) were successfully prepared by electrospinning technique, thermal treatment, and polydopamine modification. The obtained composite membranqs are composed of polymeric nanofibers with carboxylate graphene oxide nanosheets, which are anchored on the fibers by heat-induced cross linking reaction. The preparation process demonstrate eco-friendly and controllable manner. These as-formed nanocomposites were characterized by various morphological methods and spectral techniques. Due to the unique polydopamine and graphene oxide containing structures in composites, the as-obtained composite demonstrate well efficient adsorption capacity toward dye removal, which is primarily due to the specific surface area of electrospun membranes and the active polydoparnine/graphene oxide components. In addition, the composite membranes reported here are easy to regenerate. In comparison with other composite adsorbents, the preparation process of present new composite materials is highly eco-friendly and facile to operate and regulate, which demonstrates potential large-scale applications in wastewater treatment and dye removal.