Despite a lot of researches on Pulsed Laser Deposition (PLD) for film production over the years, it has largely been an unsuccessful technology because of the poor quality of laser deposited films, generally due to particle contamination. A way of improving the quality of thin films was recently developed at LPC by using MHz-repetition-rate IR laser pulses of ps-range pulse duration. As a result, Ultrafast PLD outperforms other methods in terms of surface quality, deposition rate and energy efficiency by up to three orders of magnitude. In addition, it is desirable to use short laser wavelength to more easily atomize the materials and also favor the material ablation through photochemical processes during the laser-matter interaction. An optical two-crystal tripling system has then been developed to produce high energy UV photons from a mode locked Nd:YVO4 laser (1.064 μm, 5.7 MHz, 12 ps, up to 1.5 W). A large number of UV photons can be obtained with this optical scheme providing optimum laser characteristics for efficient PLD. This is further applied to the synthesis of various high quality thin films, including polymer films and nonlinear optical films for photonic applications.