Highly oriented indium tin oxide (ITO) thin films were grown by pulsed-laser deposition (PLD) on glass and single-crystal yttria-stabilized zirconia (YSZ) substrates. The structural, electrical, and optical properties of these films were investigated as a function of oxygen partial pressure. Films were deposited at substrate temperature of 300 °C in mixed gases (12 mTorr of argon and 1–50 mTorr of oxygen) using a KrF excimer laser (248 nm and 30 ns full width at half maximum) at a fluence of 1.2 J/cm2. ITO films (300 nm thick), deposited by PLD on YSZ at 300 °C in a gas mixture of 12 mTorr of argon and 6 mTorr of oxygen, exhibit a low electrical resistivity (1.6×10−4 Ω cm) with a high transparency (∼74%) at 550 nm. ITO films deposited on both glass and YSZ substrates have been used as an anode contact in organic light-emitting diodes. A comparison of the device performance for the two substrates shows that the device fabricated on the ITO/YSZ has a higher external quantum efficiency than that of the device fabricated on the ITO glass.