This study presents a novel feedback-regulation system for highly efficient sulfur dioxide (SO₂) sensing using Pt-MoS₂ materials. The system involves the interaction between single Pt sites and adjacent S species on the MoS₂ support, where the Pt sites induce the volatilization of adjacent S species, forming S vacancy-assisted single Pt sites (Pt-Vs). These Pt-Vs then provide a feedback role by tailoring the antibonding-orbital electronic occupancy state of the Pt atoms, enhancing the adsorption of SO₂ molecules. The Pt₁-MoS₂-def sensors exhibit high SO₂ responses and a low limit of detection (3.14% to 500 ppb SO₂) at room temperature. In situ Raman, ex situ X-ray photoelectron spectroscopy, and density functional theory analysis confirm the integrity of the feedback-regulation system, which expands the electron transfer path from single Pt sites to the whole Pt-MoS₂ supports in SO₂ gas. Equipped with wireless-sensing modules, the Pt₁-MoS₂-def sensors array can realize real-time monitoring of SO₂ levels and cloud-data storage for plant growth, demonstrating the potential for optimizing plant growth conditions.This study presents a novel feedback-regulation system for highly efficient sulfur dioxide (SO₂) sensing using Pt-MoS₂ materials. The system involves the interaction between single Pt sites and adjacent S species on the MoS₂ support, where the Pt sites induce the volatilization of adjacent S species, forming S vacancy-assisted single Pt sites (Pt-Vs). These Pt-Vs then provide a feedback role by tailoring the antibonding-orbital electronic occupancy state of the Pt atoms, enhancing the adsorption of SO₂ molecules. The Pt₁-MoS₂-def sensors exhibit high SO₂ responses and a low limit of detection (3.14% to 500 ppb SO₂) at room temperature. In situ Raman, ex situ X-ray photoelectron spectroscopy, and density functional theory analysis confirm the integrity of the feedback-regulation system, which expands the electron transfer path from single Pt sites to the whole Pt-MoS₂ supports in SO₂ gas. Equipped with wireless-sensing modules, the Pt₁-MoS₂-def sensors array can realize real-time monitoring of SO₂ levels and cloud-data storage for plant growth, demonstrating the potential for optimizing plant growth conditions.