In this study, an effective approach is proposed for the controlled production of ZnO nanorod arrays that can be used in degradation of wastewater pollutants. Hydrothermal precursor solutions prepared using HMTA-different supporting ligands having different lengths and ends, which have not been tried before, allowed to control the type, size, and alignment of ZnO nanorods. Their physical properties were investigated by using X-ray diffraction patterns, Raman, FTIR and photoluminescence spectroscopies, UV/Vis Spectrophotometer, atomic force microscopy, field emission scanning electron microscopy and energy dispersive X-ray spectroscopy. Photoactivity tests were performed using methylene blue under UV/visible light and the reusability of ZnO nanorod arrays with the best properties was checked. The approach of using different supporting ligands led to different effects on the physical and photocatalytic properties. ZnO nanorod arrays gained the ZnO films, which became photoactive with UV light, the ability to benefit from visible light as well. Especially ZnO-HMTA-HMDA nanorod arrays will shed light on researchers as an effective strategy for the development of new functional nanomaterials having high photodegradation efficiency and fast kinetic.