Nanocomposites of chitosan and graphene oxide are prepared by simple self-assembly of both components in aqueous media. It is observed that graphene oxide is dispersed on a molecular scale in the chitosan matrix and some interactions occur between chitosan matrix and graphene oxide sheets. These are responsible for efficient load transfer between the nanofiller graphene and chitosan matrix. Compared with the pure chitosan, the tensile strength, and Young's modulus of the graphene-based materials are significantly improved by about 122 and 64%, respectively, with incorporation of 1 wt % graphene oxide. At the same time, the elongation at the break point increases remarkably. The experimental results indicate that graphene oxide sheets prefer to disperse well within the nanocomposites.