Nanocomposites consisting of polyvinyl alcohol (PVA) and graphitic carbon nitride nanoparticles (gC 3 N 4) were fabricated by solution casting technique. XRD has shown that the semicrystalline PVA structure is greatly affected by the incorporation of gC 3 N 4, which is confirmed by SEM images. Optical characteristics are investigated at room temperature within the wavelength range (200–1500 nm). The effect of gC 3 N 4 content on the optical band gap was studied. The optical bandgaps, direct and indirect, of gC 3 N 4 doped films, is lower than pristine PVA. Urbach’s energy increased from 0.42 eV for PVA to 0.96 eV for 14.8 wt% gC 3 N 4 doped film. The dielectric constant ε′, dielectric loss ε ″, and AC electrical conductivity σ ac at RT as a function of frequency from 100 Hz to 1 MHz, and gC 3 N 4 doping level were studied. The variation of σ ac with frequency was analyzed in view of Jonscher's universal power law. Adding gC 3 N 4 appears to enhance the σ ac of the films to higher values that candidates them in semiconductors applications. The results optical limiting indicates that the samples doped with gC 3 N 4 are highly attenuated for the laser beam of 638.2 nm. gC 3 N 4-doped PVA is a promising candidate for electronic and optoelectronic applications, especially the attenuation of laser power.