We synthesized Sn-doped In2O3 (Indium tin oxide, ITO) thin films using electrospray and spin-coating. Scanning electron microscopy, atomic force spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, Hall-effect measurement, and UV-vis spectrophotometry measurements were performed to investigate the morphological, structural, chemical, electrical, and optical properties of the electrosprayed ITO films with a sol-layer coating for surface modification. To obtain the optimum performance of the resultant ITO thin films after surface modification, we heat-treated them at four different temperatures of 450 degrees C (sample A), 550 degrees C (sample B), 650 degrees C (sample C), and 750 degrees C (sample D) using microwave heating. Surface modified ITO thin films calcined at 550 degrees C (sample B) using electrospray and spin-coating are observed to have superior resistivity (9.9 x 10(-3) 2 Ω x cm) and optical transmittance (-92.08%) owing to the improved densification of the ITO surface by spin-coating and the formation of uniform ITO thin films by electrospraying.