In this study, the thin-film vertical-type AlGaInP LEDs on Cu substrates were fabricated. By performing the epitaxial lift-off (ELO) process, the LED device can be transferred from GaAs to Cu substrate. Then the GaAs substrate was separated and the ELO-LED was completed. To overcome the drawback of crack formation in the epilayer during the ELO process, various patterned Cu substrates were designed. Moreover, the finite element method was used to simulate the stress distribution in the LED sample during the ELO process. From the simulation results, an optimum structure of patterned Cu substrate was obtained since its maximum stress can be confined to the chip edges and the stress was decreased significantly during the ELO process, resulting in an apparent reduction of crack generation after separating the GaAs substrate. This optimum patterned Cu substrate was employed for the fabrication of ELO-LED. In addition, the chemical etching process was also used to etch the GaAs substrate, and this device transferred to Cu substrate was denoted as CE-LED. Based on the measurements of device performances, the forward voltages (@350 mA) of the CE-LED and ELO-LED were measured to be 2.20 and 2.29 V, while the output powers (@350 mA) of these two devices were 49.9 and 48.2 mW, respectively. Furthermore, the surface temperatures (@350 mA) of these two samples were 46.9-48.3 and 45.2-47.0 °C, respectively. Obviously, the device characteristics of the ELO-LED are very similar to those of the CE-LED. It confirms that the design of patterned Cu substrate is very helpful to obtain the thin-film vertical-type AlGaInP LEDs. Additionally, via the ELO process, the separated GaAs substrate can be reused for production cost down.