We have developed a technology and for the first time, present here, the fabrication of continuous two-dimensionally crystallized g-C3N4 layered thin films oriented in a hexagonal lattice c-plane on glass and monocrystalline silicon substrates using chemical vapor deposition from a melamine source. Scanning electron microscopy and X-ray diffraction studies revealed that such films with a smooth surface and good crystalline quality as thick as up to 1.2 μm can be formed at a synthesis temperature of 550–625 °C. They are transparent in the visible range and demonstrate intense photoluminescence (PL) at room temperature. It was found that the band gap of the obtained material and its PL spectral range are shifting to the lower energies at high synthesis temperatures. Oriented g-C3N4 layered thin films deposited on flat solid substrates are promising for integrated electronics and optoelectronics
