Carbon nitride (C x N y ) layers with N/C ratios of 0.76±1.26 have been grown under low pressure from two organic chemical systems, namely 2,4-dichloro-6-bis(trimethylsilyl)imido-1,3,5-triazine [C 3 N 3 Cl 2 N(SiMe 3 ) 2 ] and tetramethylguanidine (C 5 H 13 N 3 ) + 2,4,6-trichloro-1,3,5-triazine (C 3 Cl 3 N 3 ). The films synthesized are transparent, well-adhered on silicon, homogeneous in morphology, and uniform in thickness. In addition, a technology has been developed for the deposition of carbon nitride powders with a N/C ratio of 1.3 as starting materials for further thermal treatment attempts in order to synthesize crystalline C 3 N 4 . At deposition temperatures between 400 and 800 C and high supersaturation of reagents in the reactor, the powders obtained exhibit nuclei of crystalline phases.