An hydrogenated nitrogen-rich graphitic carbon nitride, structurally related to the theoretical graphitic phase of C 3 N 4 , has been synthesized in a bulk wellcrystallized form. This new material was prepared by thermal decomposition of thiosemicarbazide up to 600°C at ambient pressure under nitrogen flow. Its composition was determined by elemental combustion analysis. Powder X-ray diffraction, infrared spectroscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy and C
13MAS NMR characterizations were performed. This material can be schematically described with a two-dimensional framework and a composition close to C 3 N 4.17 H 1.12 . In this nitrogen-rich material, C 3 N 3 voids are fully occupied by water molecules which are strongly trapped into the material. A loss of crystallinity associated with a modification of the thermal behaviour is observed when the amount of trapped molecules decreases in the graphitic material, order being damaged both between and in the graphitic planes.