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A procedure was developed for preparing bulk carbon nitride crystals from a polymeric α-C3N4.2 at high pressure and temperature in the presence of seeds of crystalline carbon nitride films prepared by a high voltage discharge plasma combined with pulsed laser ablation of graphite target. The samples were evaluated by x-ray photoelectron spectroscopy (XPS), infrared (IR) spectroscopy, Auger electron spectroscopy (AES), secondary-ion mass spectrometry (SIMS), scanning electron microscopy (SEM) and x-ray diffraction (XRD). Notably, XPS studies of the film composition before and after thermobaric treatments demonstrate that the nitrogen composition in α-C3N4.2 material initially containing more than 58% nitrogen decreases during the annealing process and reaches a common, stable composition of ~45%. The thermobaric experiments were performed at 10-77 kbar and 350-1200 °C.