Zirconium/titanium/chitosan (Zr/Ti/CHT) composite catalysts were synthesized by sol-gel method using different chitosan amounts (5–20 wt.%) and their activity in the photocatalytic degradation of Orange II dye was evaluated for the first time. The results were compared with Zr/Ti, Zr/CHT and Ti/CHT catalysts. The composite catalysts were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy, scanning electron microscopy and X-ray photoelectron spectroscopy analysis. XRD analysis revealed that the Zr/Ti/CHT composite catalyst showed high crystallinity of anatase TiO2 phase. Photocatalytic experiments showed that adding CHT into the catalyst structure increased the photocatalytic degradation under visible light irradiation. Also, the first-order reaction rate constant, kapp, was calculated using the Langmuir–Hinshelwood (L-H) equation. The kapp values were found to be 0.009, 0.0013, 0.012 and 0.014 min−1 for Zr/Ti, Zr/CHT, Ti/CHT and Zr/Ti/CHT, respectively. According to stability tests, after the first cycle Orange II dye degradation was found to be 95%, while it was 37% after the fifth cycle. The results showed that the composite catalyst could be used several times for Orange II dye degradation.