Single-atom catalysts (SACs) hold great promise in highly sensitive and selective gas sensors due to their ultrahigh atomic efficiency and excellent catalytic activity. However, due to the extremely high surface energy of SACs, it is still a huge challenge to synthesize a stable single-atom metal on sensitive materials. Here, we report an atomic layer deposition (ALD) strategy for the elaborate synthesis of single-atom Pt on oxygen vacancy-rich Fe 2 O 3 nanosheets (Pt−Fe 2 O 3 −V o ), which displayed ultrafast and sensitive detection to H 2 , achieving the stability of Pt single atoms. Gassensing investigation showed that the Pt−Fe 2 O 3 −V o materials enabled a significantly enhanced response of 26.5−50 ppm of H 2 , which was 17-fold higher than that of pure Fe 2 O 3 , as well as ultrafast response time (2 s), extremely low detection limit (86 ppb), and improved stability. The experimental and density functional theory (DFT) studies revealed that the abundant oxygen vacancy sites of Fe 2 O 3 contributed to stabilizing the Pt atoms via electron transfer. In addition, the stabilized Pt atoms also greatly promote the electron transfer of H 2 molecules to Fe 2 O 3 , thereby achieving an excellent H 2 sensing performance. This work provides a potential strategy for the development of highly selective and stable chemical sensors.