Atomically dispersed metal catalysts can maximize the utilization of metals and provide unique chemical properties for catalytic reactions. However, the stabilities of high-loading metal clusters on solid supports are still under dispute, because small clusters are prone to agglomerate into larger particles at high temperature. Here, we prepared thermally stable highly dispersed Pt species immobilized by bridging Zn2+ sites and silanol groups (Si-OH) on self-pillared silicalite-1 zeolite nanosheets (SP-S-1). The rotationally overgrown zeolite sheet-like structure provided a high specific surface area and abundant Si-OH, which favored atomically dispersed active sites with ZnOx-Si nanoclusters. The as-prepared PtZn/SP-S-1 exhibited a high specific activity of 1.23 molC3H6·gcatal–1·h–1 at 580 °C with propylene selectivity up to 99%. Moreover, no obvious deactivation was observed after 90 h on stream under a weight hourly space velocity of 15 h–1. The self-pillared nanosheet-supported metal catalysts provide prospective guidance for high-temperature catalysis.