Novel two-dimensional ZnO/Ti₃C₂T_x hybrid photocatalysts with modified surface areas were prepared using a simple calcination technique. The microstructures, crystalline features, and bonding states of the ZnO structure-covered Ti₃C₂T_x MXenes were closely characterized using various tools. The photoluminescence intensity of the hybrid photocatalyst was greatly reduced compared to the pristine ZnO, while its Brunauer-Emmett-Teller (BET) surface area increased by more than 100 times. Under solar light illumination, the photocatalytic degradation efficiency of the hybrid photocatalyst for organic pollutants (MO, RhB) appeared to be three-fold larger as compared to pristine ZnO. The superb photocatalytic performance of the photocatalyst was attributed to several factors, such as ideal band alignment, Schottky barrier formation, and large surface area. Moreover, the ZnO/Ti₃C₂T_x hybrid photocatalyst showed excellent cycling stability. These results suggest that the novel hybrid structure may be a potential candidate for removing organic pollutants in wastewater.