Self-nanostructured ZnO:Al conductive layers consisting of [112̅0] oriented domains were coated by a conformal TiO2 thin film and sensitized by 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin (TCPP) to be used as transparent conductive electrodes in dye-sensitized solar cells. In addition to the higher surface availability due to the nanopatterning, the TCPP surface density increases by 330% (UV−vis) with respect to a flat conventional substrate thanks to a more dense molecular arrangement, as evidenced by combining high-resolution X-ray photoelectron spectroscopy and atomic force microscopy. Furthermore, the presence of zinc atoms in the TiO2 overlayer (Ti(:Zn)O2) crucially influences the electronic properties of the assembled TCPP. As a consequence of the orbitals' rearrangement attributed to the presence of zinc, a significant quenching of luminescence is observed in the emission spectra of TCPP …