In this work, we report the effect of cetyl trimethyl ammonium bromide (CTAB), ethyl di-tetra amine (EDTA) and polyacrylamide as surfactants on synthesis of zinc oxide for photocatalytic application. The ZnO nanoparticles were synthesized with and without the surfactants and characterized using powder X-ray diffraction (PXRD), and Fourier transform infrared spectroscopy (FTIR). In addition to this, the morphology of zinc oxide prepared in the absence and presence of these surfactants investigated through scanning electron microscopy (SEM). As confirmed from XRD and FTIR characterization results, the use of different surfactants did not affect the composition of ZnO nanomaterials. The photocatalytic activities were investigated by the degradation of methylene blue (MB) dye under sunlight irradiation. To optimize the effects of operational parameters, the study was carried out as a function of dye concentration, catalyst dose, and pH on the degradation efficiency of the photocatalysts. The optimum values of catalyst dose, dye concentration and pH of solution were found to be 0.09 g, 5 mg/L and 10, respectively. The ZnO nanomaterials prepared with CTAB surfactant showed highest degradation efficiency of 98% indicating potential application for practical decontamination of wastewater from toxic organic pollutants. KEY WORDS: Surfactants, Zinc oxide nanoparticles, Photocatalysis, Methylene blue Bull. Chem. Soc. Ethiop. 2024, 38(4), 923-935. DOI: https://dx.doi.org/10.4314/bcse.v38i4.9