This paper reports the synthesis of Fe-titanate nanotubes by means of the conventional ion-exchange method with iron nitrate solutions. As the iron-rich nanotubes were found to contain the catalyst precursor intrinsically dispersed in their structures, the unprecedented possibility of using this kind of materials for building carbon nanostructures, firmly attached at the surface of the forming TiO₂ nanoparticles, was verified. The catalytic decomposition of ethylene, used as a carbon source, was performed at a relatively high temperature (750 °C) when the nanotubes undergo an irreversible phase transformation to form anatase and rutile nanoparticles. Due to the different amounts of Fe ions in the nanotubes, distinct types of carbon/TiO₂ hybrid interfaces were formed, ranging from amorphous (lower Fe³⁺ concentration) to the more crystalline graphitic domains (higher Fe³⁺ concentrations), as documented by the microstructure of the treated samples. The present approach is of potential interest for (photo)catalytic and energy conversion/transport applications.