The strong metal-support interaction exerts a significant influence on the catalytic performance of the metal active site. This paper describes the modulation of the coverage of TiOx on the Pt nanoparticles via the pretreatment atmosphere, and its influence of the catalytic performance for propane dehydrogenation. The direct reduction in H2 at 600 °C of the Pt/TiO2-Al2O3 catalyst induces partial coverage of the Pt nanoparticles by TiOx. This partial coverage with TiOx leads to higher electron density over platinum than catalysts treated through air calcination followed by reduction, which can enhance the selectivity of propylene. Furthermore, the presence of TiOx in the catalysts can promote C–H activation during propane dehydrogenation. Eventually, this synergistic catalyst presents a high formation rate of propylene (141.1 mmol·gcat-1·h−1) and propylene selectivity of ∼ 91 % with a low deactivation rate of 0.09 h−1. This study unveils an effective approach to modulate the catalytic performance of metals supported on oxides based on metal-support interaction.