We developed a simple, versatile method of integrating hybrid thin films of reduced graphene oxide (RGO) nanosheets with multiwalled carbon nanotubes (MWNTs) via LbL assembly. This approach involves the electrostatic interactions of two oppositely charged suspensions of the RGO nanosheet with MWNTs. This method affords a hybrid multilayer of graphenes with excellent control over the optical and electrical properties. Moreover, the hybrid multilayer exhibits a significant increase of electronic conductivity after the thermal treatment, producing transparent and conducting thin films possessing a sheet resistance of 8 kOmega/sq with a transmittance of 81%. By taking advantage of the conducting network structure of MWNTs, which provides an additional flexibility and mechanical stability of RGO nanosheets, we demonstrate the potential application of hybrid graphene multilayer as a highly flexible and transparent electrode. Because of the highly versatile and tunable properties of LbL-assembled thin films, we anticipate that the general concept presented here offers a unique potential platform for integrating active carbon nanomaterials for advanced electronic, energy, and sensor applications.

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