Despite great recent progress with graphene based materials, the development of strong and cost efficient multifunctional graphene filled polymer composites has not yet to be achieved A key challenge in the fabrication of nanoplatelet filled polymer composites is the ability to realize the nanometer-level dispersion and the planar orientation of nanosheets in polymer matrices In this report, ultrathin multilayer (PVA/GO)(n) films were successfully fabricated by bottom-up layer by-layer (LBL) assembly of poly(vinyl alcohol) (PVA) and exfoliated graphene oxide (GO), in which exfoliated GO nanosheets were used as the building blocks Typical tapping-mode atomic force microscope (AFM) and field emission scanning electron microscope (FESEM) Images demonstrate an ordered arrangement of organic and inorganic layers A significant enhancement of mechanical properties has been achieved, that is a 98 7% improvement of elastic modulus (E-r) and a 240 4% Increase of hardness This may be attributed to the well-defined layered architecture with high degree of planar orientation and nanolevel assemblies of GO nanosheets in the polymer matrices