Laser ablation of metal thin films draws attention as a fast means of clean micropatterning. In this study, we attempt to remove only the metal thin film layer selectively without leaving thermal damage on the underneath substrate. Specifically, our single-pulse ablation experiment followed by two-temperature analysis explains that selective ablation can be achieved for gold (Au) films of 50-100 nm thickness by the lift-off process induced as a result of vaporization of the titanium (Ti) interlayer with a strong electron-phonon coupling. With increasing the film thickness comparable to the mean free path of electrons (100 nm), the pulse duration has to be taken shorter than 10 ps, as high-temperature electrons generated by the ultrashort pulses transfer heat to the Ti interlayer. We verify the lift-off ablation by implementing millimeters-scale micropatterning of optoelectronic devices without degradation of optical properties.</p>