Free-standing hybrid films of graphene oxide (GO) and titanium dioxide nanotubes (TNT) were prepared trough a bar coating and drying method from GO-based dispersions. Successful chemical functionalization of the nanotubes with allyltriethoxysilane as a linker is confirmed by XPS and Raman spectroscopy. These resulting functionalized nanotubes were then used to prepare self-assembled hybrid films with GO in aqueous suspension. These hybrid films exhibit outstanding mechanical properties. The Young's modulus was as high as similar to 10 GPa (38% higher than the pristine graphene oxide film) and an ultimate tensile strength around similar to 40 MPa. The method presented here is versatile, and it can be easily coupled to fabricate other graphene-based hybrid films for applications, such as fuel-cells, photocatalysis, filters, amongst others.