Modification of TiO2 is one of the techniques used to enhance its photodegradation efficiency and to make it visible-light-active. In this study, Mo-doped TiO2 nanoparticles were synthesized using a fast sol-gel technique, and then coated on granular activated carbon (GAC) as both substrate and adsorbent to obtain Mo:TiO2/GAC composite. The fabricated composite was characterized using powder XRD, SEM, EDAX, FTIR, and BET analysis. Then the composite was applied to photodegrade volatile organic compounds (VOCs) under both UV and visible light irradiation. The characterization results showed high crystallinity and purity. Mo:TiO2/GAC composite had higher photodegradation efficiency compared with bare TiO2 and bare GAC. Moreover, studying operational parameters showed that the optimum condition for photodegradation efficiency of VOCs was at flowrate of 1 l/min, VOCs concentration of 20 ppm, and light intensity of 400 and 600 W/m2 for UV and visible light respectively. The results suggest that Mo:TiO2/GAC is a visible-light-active composite and can be acceptably used to decompose VOCs under visible light with adequate efficiency and without the generation of harmful by-products such as O3 as compared with UV.