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Gallium nitride (GaN), as a promising alternative semiconductor to silicon, is of well-established use in photoelectronic and electronic technology. However, the vulnerable GaN surface has been a critical restriction that hinders the development of GaN-based devices, especially regarding device stability and reliability. Here, we overcome this challenge by converting the GaN surface into a gallium oxynitride (GaON) epitaxial nanolayer through an in-situ two-step "oxidation-reconfiguration" process. The oxygen plasma treatment overcomes the chemical inertness of the GaN surface, and the sequential thermal annealing manipulates the kinetic-thermodynamic reaction pathways to create a metastable GaON nanolayer with wurtzite lattice. This GaN-derived GaON nanolayer is a tailored structure for surface reinforcement and possesses several advantages, including wide bandgap, high thermodynamic stability, and large valence band offset with GaN substrate. These enhanced physical properties can be further leveraged to enable GaN-based applications in new scenarios, such as complementary logic integrated circuits, photoelectrochemical water splitting, and ultraviolet photoelectric conversion, making GaON a versatile functionality extender.