Ni-doped FTO thin films were prepared by aerosol-assisted chemical vapor deposition (AACVD) using monobutyltin trichloride (MBTC) as tin source, ammonium fluoride (NH4F) as fluorine source, methanol as solvent, and nickel chloride hexahydrate (NiCl2·6H2O) as nickel source. The optical and electrical properties of FTO thin films were characterized and analyzed by spectrophotometer, four-probe resistor meter and Hall effect tester. The electronic structure of doped system was calculated based on first principles as well. The results indicate that the Ni-doped FTO thin films are tetragonal rutile structure, and the conductivity is improved. When Ni/Sn is 2%(atomic fraction), the quality factor ΦTC reaches 3×10-2 Ω-1, the resistivity ρ is 3.79×10-4 Ω·cm, the average transmittance of visible light is about 80%, the carrier concentration n is 6.88×1020 cm-3, and the mobility μ is 13.31 cm2·V-1·s-1.