Single crystalline nanomembranes (NMs) represent a new embodiment of semiconductors having a two-dimensional flexural character with comparable crystalline perfection and optoelectronic efficacy. In this Letter, we demonstrate the preparation of GaN NMs with a freestanding thickness between 90 to 300 nm. Large-area (>5 × 5 mm(2)) GaN NMs can be routinely obtained using a procedure of conductivity-selective electrochemical etching. GaN NM is atomically flat and possesses an optical quality similar to that from bulk GaN. A light-emitting optical heterostructure NM consisting of p-GaN/InGaN quantum wells/GaN is prepared by epitaxy, undercutting etching, and layer transfer. Bright blue light emission from this heterostructure validates the concept of NM-based optoelectronics and points to potentials in flexible applications and heterogeneous integration.