This work investigated the efficiency of polyethylene terephthalate (PET) as support material for TiO2 films in the photocatalytic degradation of red Bordeaux and yellow tartrazine dyes. The optimum operating conditions were determined by a factorial design, which resulted after 180 min of treatment in degradations of 99.5% and 99.1% for the UVC/H2O2/TiO2Sup and solar/H2O2/TiO2Sup systems, respectively. For the kinetic study, the experimental data fitted to the pseudo-first-order model and the calculated kinetic constants (k) values were 0.03 min−1 for the UVC/H2O2/TiO2Sup system and 0.0213 min−1 for the system solar/H2O2/TiO2Sup. It was verified that TiO2 supported in the PET remained with high degradation efficiency even after five cycles of reuse, indicating a good stability of the photocatalyst in the support. A significant reduction of TOC content was also observed along the reaction time. The phytotoxicity bioassay with Lactuca sativa demonstrated that after treatment with UVC/H2O2/TiO2Sup and solar/H2O2/TiO2SUP, an increase in IC50 and consequently lower toxicity was observed.