Layered double hydroxide Ti-Zn-CO3 was synthesized by the co-precipitation method with a molar ratio of 2. The synthesized material was characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), thermal analysis (TGA/DTG), UV–vis diffuse reflection spectroscopy (DRS), and Scanning Electron Microscopy (SEM). The photocatalytic degradation of Trypan Blue (TB) and Naphthol Green B (NGB) dyes from aqueous solutions under UV irradiation was investigated. The effects of contact time, photocatalyst dose, dye concentration, solution pH, scavenger effect, and regeneration of catalyst were investigated. The kinetic study showed that the equilibrium was reached within 30 min and 40 min for TB and NGB dyes, respectively, with photodegradation efficiency of around 91% and 83% for TB and NGB dyes, respectively, for dye concentration of 25 mg∙L−1, and the pseudo-first order showed good agreement with the reaction. The optimum photocatalyst dose is 20 mg (1 g∙L−1) and 30 mg (1.5 g∙L−1) for TB and NGB dyes, respectively, and the optimal pH of reaction was found to be 7 for both TB and NGB dyes. This study was established to highlight the photodegradation performance of the prepared catalyst Ti-Zn-CO3 for the degradation of (TB and NGB) dyes chosen as pollutants, and the fact that it can be used many times, which has an economical effect. This mean that the prepared sample is a potential catalyst with good photocatalytic activity, stability, and reusability.