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Vertical light-emitting diodes (LEDs) were successfully fabricated by a chemical lift-off process using a selectively etchable CrN buffer layer. The novel CrN metallic layer worked well as a buffer layer for growth of the GaN LED and was etched out clearly during selective chemical etching. The vertical LED by chemical lift-off showed very good current-voltage performance with low series resistance of 0.65 Omega and low operated voltage of 3.11 V at 350 mA. Also, this device could be operated at a much higher injection forward current (1118 mA at 3.70 V) by thermally conductive metal substrate which enabled the high current operation with excellent heat dissipation.