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In this data article, the normalized emission and excitation spectra, the ultraviolet-visible (UV–vis) absorption spectra, and the X-ray photoelectron spectroscopy (XPS) of bulk-powders and nano-structured graphitic C3N4 (g-C3N4) were presented, which are helpful to get insight into the crystal and electronic structures of g-C3N4, especially on determining the energy levels and the mechanisms of luminescence originating from electron transitions. This data article is related to our recent publication (He et al., in press) [1]. The absorption, excitation and emission spectra are vital to illustrate the optoelectronic performances in terms of photoluminescence, photocatalysis, electroluminescence, etc., from the viewpoint of electron transitions intrinsically. Keywords: Graphitic C3N4, Luminescence spectra, Absorption spectra, X-ray photoelectron spectroscopy (XPS)