The ilmenite-hematite (1 -x) FeTiO 3 Á xFe 2 O 3 solid solution system is considered to be a novel material for spin-electronics, microelectronics, hightemperature electronics, and radhard electronics. This paper focuses on thin films of composition x = 0.33 grown on (100) MgO single-crystal substrates using pulsed-laser deposition (PLD) under different argon-oxygen mixtures. The surface of the MgO was found to possess MgO 2 crystals, yielding an orientation relationship, [001] MgO k [011] MgO 2 and (100)MgO k (110) MgO 2 . The structural characterizations show that the films are crystalline and homogeneous without any secondary phase. The films show a weak and inclined (1120) growth epitaxy. A bandgap of 3.4-3.7 eV was obtained for these films from optical measurements carried out in the UV-visible region. Electrical measurements confirmed the semiconducting behavior. However, the resistivity was found to increase substantially on the slightest addition of oxygen into the chamber.