A series of thermally stable and highly luminescent cyclometalated tetradentate ligand-containing gold(III) compounds was designed and synthesized. The cyclometalated tetradentate ligand-containing gold(III) compounds can be used as light-emitting material for fabrication of light-emitting devices. The cyclometalated tetradentate ligand-containing gold(III) compounds can be deposited as a layer or a component of a layer using a solution-processing technique or a vacuum deposition process. The cyclometalated tetradentate ligand-containing gold(III) compounds are robust and can provide electroluminescence with high efficiency and brightness. More importantly, the vacuum-deposited OLEDs demonstrate long operational stabilities with half-lifetime of over 29,700 hours at 100 cd m−2.