Carbon doped ZnO nanoparticles have been synthesized from the thermal decomposition of Zinc citrate precursor. The precursor was synthesized from semi-solid paste and then subjected to calcination at 700 °C to produce ZnO nanoparticles. The precursor and ZnO were characterized by Fourier Transform Infrared Spectroscopy, UV–visible (UV–Vis) spectra, Transmission Electron Microscope, Field Emission Scanning Electron Microscope, Energy Dispersive Analysis by X-ray (EDAX), X-ray powder diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The results ensured the formation of hexagonal 2D-ZnO nanoparticles with a layer thickness of 25 nm. The optical band gap of ZnO was determined and found to be 2.9 eV, which is lower than the bulk. Photocatalytic degradation of Fluorescein dye as an anionic dye and Rhodamine B as a cationic dye was evaluated via C-ZnO NPs under UV irradiation. ZnO displayed 99% degradation of Fluorescein dye after 240 min and a complete photocatalytic degradation of Rhodamine B dye after 120 min under UV irradiation.