Abstract Multiwalled carbon nanotube/TiO2 multilayer nanocomposite was successfully deposited on the fluorine-doped tin oxide (FTO) glass via layer-by-layer assembly technique to modify interfacial contact between the FTO surface and nanocrystalline TiO2 layer as well as carbon nanotube/TiO2 contacts in photoanode of dye sensitized solar cell. Using this approach, binder-free interfacial thin film was developed with nonagglomerated, well-dispersed MWCNTs on FTO and into TiO2 matrix and with maximum covering of TiO2 nanoparticles on MWCNTs. Introduction of MWCNTs/TiO2 interfacial layer into the TiO2 photoanode increased short circuit current density (Jsc) from 11.90 to 17.25 mA/cm2 and open circuit voltage (Voc) from 730 mV to 755 mV, whereas there was no notable change in the fill factor (FF). Consequently, power conversion efficiency (η) was enhanced from 5.32 to 7.53 %, yielding a 41.5 % enhancement. The results suggest that our simple strategy can integrate reduction of back electron reaction at FTO/TiO2 interface with the effective charge transport ability of carbon nanotubes and possessing high surface area for efficient dye loading.