N-doped ZnO beads (NZB) and N-doped TiO2 beads (NTB) were synthesized via a modified sol–gel technique utilizing chitosan (CS)/polyvinyl alcohol (PVA) hydrogel beads as basic support for photocatalyst. Urea was used as a source of nitrogen in the preparation of N-doped ZnO beads, while ammonium acetate, CH3COONH4, was used as a nitrogen source in the production of N-doped TiO2 beads. The characteristics of synthesized beads were identified by scanning electron microscope (SEM), X-ray photoelectron spectroscopy analysis (XPS), X-ray diffraction (XRD), N2 adsorption–desorption isotherms, BET surface area, Fourier transform infrared (FT-IR) measurements, and diffuse reflectance spectroscopy (DRS) studies. The use of the nitrogen doping method for photocatalyst was performed to adjust the bandgap and electrical properties of ZnO and TiO2 by establishing acceptor defects. NZB and NTB with the intrinsic donor defect of oxygen vacancy and the nitrogen-to-oxygen acceptor defect could be activated by a less-energy UV consumption for efficient pollutant degradation. The results indicated that the as-synthesized NZB achieved much higher degradation activity than NTB, commercial ZnO, and TiO2 in the decomposition of a binary mixture composed of ammonia and phenol under UV light irradiation.