Device quality indium tin oxide (ITO) films are deposited on glass substrates and ultra-thin diamond-like carbon films are deposited as a buffer layer on ITO by a pulsed Nd:YAG laser at 355 nm and 532 nm wavelength. ITO films deposited at room temperature are largely amorphous although their optical transmittances in the visible range are > 90%. The resistivity of their amorphous ITO films is too high to enable an efficient organic light-emitting device (OLED), in contrast to that deposited by a KrF laser. Substrate heating at 200℃ with laser wavelength of 355 nm, the ITO film resistivity decreases by almost an order of magnitude to 2×10 -4 Ω cm while its optical transmittance is maintained at > 90%. The thermally induced crystallization of ITO has a preferred <111> directional orientation texture which largely accounts for the lowering of film resistivity. The background gas and deposition distance, that between the ITO target and the glass substrate, influence the thin-film microstructures. The optical and electrical properties are compared to published results using other nanosecond lasers and other fluence, as well as the use of ultra fast lasers.Molecularly doped, single-layer OLEDs of ITO/(PVK+TPD+Alq3)/Al which are fabricated using pulsed-laser deposited ITO samples are compared to those fabricated using the commercial ITO. Effects such as surface texture and roughness of ITO and the insertion of DLC as a buffer layer into ITO/DLC/(PVK+TPD+Alq3)/Al devices are investigated. The effects of DLC-on-ITO on OLED improvement such as better turn-on voltage and brightness are explained by a possible reduction of energy barrier to the hole injection from ITO into the light-emitting layer.