Multi-walled carbon nanotubes/reduced graphene oxide (MWCNT/rGO) hybrid films have attracted increasing massive attention due to their unique advantages such as high conductivity, superior mechanical property and thermal properties. In this work, a novel, facile and low cost method was developed to fabricate the MWCNT/rGO flexible ultrathin hybrid films with the thickness of about 55 nm. These hybrid films can be fabricated repeatedly through layer-by-layer exfoliation on the surface of liquids, and transferred to various substrates. The devices based on MWCNT/rGO hybrid films offer a unique platform for integrating carbon nanomaterials for advanced electronics, energy, and sensor applications.