Visible-light-enhanced TiO2 nanocatalysts doped with Cu and Fe were synthesized using the sol-gel method to investigate their performance in degrading gaseous benzene. The structure and morphology of mono- and co-doped TiO2 (i.e., Cu/Fe-TiO2, Cu-Fe-TiO2) were characterized using SEM, EDS, XRD, BET, Raman, UV-vis-DRS, and XPS techniques. The results indicated that the presence of Cu/Fe mono- and co-doped TiO2 leads to the formation of an anatase phase similar to pure TiO2. Furthermore, the introduction of Cu/Fe enhanced the presence of lattice defects and increased the specific surface area of TiO2. This enhancement can be attributed to the increase in oxygen vacancies, especially in the case of Cu-Fe-TiO2. Additionally, Cu-Fe-TiO2 showed a higher concentration of surface-bound hydroxyl groups/chemically adsorbed oxygen and a narrower bandgap than pure TiO2. Consequently, Cu-Fe-TiO2 exhibited the highest photocatalytic performance of 658.33 μgC6H6/(g·h), achieving a benzene degradation rate of 88.87%, surpassing that of pure TiO2 (5.09%), Cu-TiO2 (66.92%), and Fe-TiO2 (59.99%). Reusability tests demonstrated that Cu-Fe-TiO2 maintained a high benzene degradation efficiency of 71.4%, even after five experimental cycles, highlighting its exceptional stability and reusability. In summary, the addition of Cu/Fe to TiO2 enhances its ability to degrade gaseous benzene by prolonging the catalyst's lifespan and expanding its photoresponse range to include visible light.