Wastewater from the textile industry is chronic and hazardous for the human body due to the presence of a variety of organic dyes; therefore, its complete treatment requires efficient, simple, and low cost technology. For this purpose, we grew ZnO microstructures in the presence of psyllium husk, and the role of psyllium husk was to modify the surface of the ZnO microstructures, create defects in the semiconducting crystal structures, and to alter the morphology of the nanostructured material. The growth process involved a hydrothermal method followed by calcination in air. Additionally, the psyllium husk, after thermal combustion, added a certain value of carbon into the ZnO nanomaterial, consequently enhancing the photocatalytic activity towards the degradation of methylene blue. We also investigated the effect of varying doses of photocatalyst on the photocatalytic properties towards the photodegradation of methylene blue in aqueous solution under the illumination of ultraviolet light. The structure and morphology of the prepared ZnO microstructures were explored by scanning electron microscopy (SEM) and powder X-ray diffraction (XRD) techniques. The degradation of methylene blue was monitored under the irradiation of ultraviolet light and in the dark. Also, the degradation of methylene blue was measured with and without photocatalyst. The photodegradation of methylene blue is highly increased using the ZnO sample prepared with psyllium husk. The photodegradation efficiency is found to be approximately 99.35% for this sample. The outperforming functionality of psyllium-husk-assisted ZnO sample is attributed to large surface area of carbon material from the psyllium husk and the synergetic effect between the incorporated carbon and ZnO itself. Based on the performance of the hybrid material, it is safe to say that psyllium husk has high potential for use where surface roughness, morphology alteration, and defects in the crystal structure are vital for the enhancing the functionality of a nanostructured material. The observed performance of ZnO in the presence of psyllium husk provides evidence for the fabrication of a low cost and efficient photocatalyst for the wastewater treatment problems.