Abstract Pt‐based catalysts have been widely investigated in propane dehydrogenation (PDH) owing to their high activity in CH activation, while it suffers from Pt sintering and coke deposition. We develop a transition metal Fe and zeolite support synergistic‐modified method to realize the highly dispersed and stable Pt species inside zeolite over Pt/Fe‐silicate‐1. And it shows the excellent PDH performance with propylene generation rate of 51.6 mol C 3 H 6 g Pt −1 h −1 and low deactivation rate constant k d of 0.017 h −1 as well as a high TOF Pt of 37.6 s −1 at 550°C. The systematic characterizations reveal the isolated Fe 3+ species could significantly improve Pt dispersity and regulate Pt electronic density to realize a more positive Pt δ+ species inside Silicalite‐1 pore. And the further in situ DRIFTS experiments demonstrate that the synergistic effect between the appropriate acidic Fe sites and the highly dispersed Pt δ+ species around Fe species are responsible for the superior PDH performance.