Poly(vinyl alcohol)(PVA)/graphene oxide (GO) nano-composite hydrogel beads were prepared by in-situ chemical cross-linking for the purpose of Pb2+ removal of heavy metal waste water, while GO was functionalized with carboxyl-silane coupling agent (CSA). It was found that the red-shift of O-H stretching vibration suggested the existence of hydrogen bonding interaction among molecules of PVA, CSA and GO layers, and relatively high intercalation ratio can be achieved. Compared with the XRD pattern of GO, the diffraction peaks of GO-CSA sample shifted to lower angles and the completely exfoliated state of GO formed for the GO-CSA/PVA sample. Both the GO-CSA and GO-CSA/PVA samples exhibited a significant increase in the average layer thickness, and the stacking of each layer is much more weakened, exhibiting a wrinkled, transparent and almost monolayer dispersion state, which led to a good dispersion of GO in the PVA matrix. With increasing GO-CSA content, the shear storage modulus and effective network density of the hydrogel increased first, reaching maximum at 0.5 wt% GO-CSA, and then decreased. Much more uniform and dense porous network structure formed, leading to the remarkable increase of the strength and toughness of the hydrogel. Pb2+ adsorption capacity of the hydrogel increased with GO-CSA content, while Langmuir isotherm fitted well with the experimental data, indicating homogeneous nature of monolayer adsorption of Pb2+. The adsorption was mainly controlled by the intraparticle diffusion, and belonged to the second-order kinetic model, indicating chemical adsorption with ion-exchange mechanism.