In the present work, zirconyl oxychloride (ZOC) thin films were prepared by using the thermal evaporation technique under a vacuum of 5×10−6 Torr. The surface and crystalline investigation of the prepared films were done by using a scanning electron microscope and X‐ray diffraction technique. The optical absorption coefficient was evaluated to find the type of transition which is indirectly allowed with an energy gap value of 3.45 eV. The photoresponse characteristics of the In/ZOC/In and Cu/ZOC/In diodes were examined by transient photocurrent measurements. Besides, ZOC, In/ZOC/In and Cu/ZOC/In was also used as a photocatalyst for an LBR textile dye removal under various conditions. Moreover, the photocatalytic degradation of aqueous LBR dye with the prepared catalysts was investigated under UV‐light irradiation. The results confirmed that Cu/ZOC/In photocatalyst is superior over the known photocatalyst and has high stability and reusability.