TiO2-supported clinoptilolites (TiO2/clinoptilolites) were successfully synthesized with controlled crystal phase and particle size via hydrothermal method to enhance photocatalytic performance of TiO2. The effects of various parameters including temperature, acidity and concentration of Ti-containing solutions on the particle size, crystal phase and agglomeration of TiO2 supported on clinoptilolite were investigated thoroughly by characterizations of X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, scanning electron microscope (SEM), transmission electron microscope (TEM), BET isotherm, UV–visible (UV–vis) spectrophotometer and Malvern zetasizer. The results demonstrate that increasing temperature and strengthen acidity are beneficial to enhance the crystallinity and particle size of supported TiO2. Increase in acidity also leads to more uniform distribution of TiO2 on the surface of clinoptilolite. The TiO2 nano-crystals deposited on the surface of clinoptilolite, exhibit rutile or anatase phase, strongly depending on the preparation procedure. The resultant TiO2/clinoptilolites could be used as photo-catalysts for the degradation of crystal violet (CV) dye in aqueous solution, showing a higher photo-catalytic activity with 89% degradation within 100 min. The effect of operational parameters, such as pH values of reaction media, dose of used catalyst, and concentration of CV dye on the CV degradation performance were investigated, in which the kinetics of CV dye degradation was found to follow the pseudo-first order kinetic model.