Nonlinear optical films of potassium titanyl phosphate (KTiOPO4, or KTP) have been, for the first time, fabricated by pulsed excimer laser deposition on several substrates such as sapphire, Si(100) crystals, and fused quartz slides. The properties of the deposited KTP films, such as the chemical stoichiometry, crystallinity, effective index of refraction, and Raman response, have been extensively characterized. All of the results match die values of KTP crystals. The nonlinear optical property of the second harmonic generation of the films has been evaluated, showing a high efficiency comparable to a bulk value of KTP crystals. It is suggested that the success of this deposition relies on the transient congruent process generated by a pulsed UV laser beam.