Substitutional doping of framework heteroatoms in photocatalysts is one of the approaches for harvesting visible light. The present work aims to utilize the visible light for photocatalytic degradation of organic pollutant by tailoring the bandgap energy of Li2VPO6 through nitrogen doping. Li2VPO6 and N-doped Li2VPO6 are prepared by solidstate method. These materials were characterized by powder X-ray diffraction, energy-dispersive spectra, Raman spectra,UV–Vis diffuse reflectance spectra(UV–Vis DRS), and31 P MAS NMR. The absorption edge of N-doped Li2VPO6 is shifted to longer wavelength region considerably. The photocatalytic activity was tested against the degradation of methylene blue. The higher visible light photocatalytic activity of N-doped Li2VPO6 compared to pristine Li2VPO6 was discussed. The catalysts are stable even after fourth cycle of photodegradation. Substitutional doping of framework heteroatoms in photocatalysts is one of the approaches for harvesting visible light. The present work aims to utilize the visible light for photocatalytic degradation of organic pollutants by tailoring the bandgap energy of Li2VPO6 through nitrogen doping. Li2VPO6 and N-doped Li2VPO6 are prepared by solidstate method. These materials were characterized by powder X-ray diffraction, energy-dispersive spectra, Raman spectra, UV-Vis diffuse reflectance spectra (UV- Vis DRS), and31 P MAS NMR. The absorption edge of N-doped Li2VPO6 The photocatalytic activity was tested against the degradation of methylene blue. The higher visible light photocatalytic activity of N-doped Li2VPO6 compared to pristine Li2VPO6 was discussed. The catalysts are stable even after fourth cycle of photodegradation.