In heterogeneous catalysis, supports play a crucial role in modulating the geometric and electronic structure of the active metal phase for optimizing the catalytic performance. A γ-Al2O3 nanosheet that contains 27% pentacoordinate Al(3+) sites can nicely disperse and stabilize raft-like Pt-Sn clusters as a result of strong interactions between metal and support. Consequently, there are strong electronic interactions between the Pt and Sn atoms, resulting in an increase in the electron density of the Pt sites. When used in the propane dehydrogenation reaction, this catalyst displayed an excellent specific activity for propylene formation with >99% selectivity, and superior anti-coking and anti-sintering properties. Its exceptional ability to maintain the high activity and stability at ultrahigh space velocities further showed that the sheet construction of the catalyst facilitated the kinetic transfer process.