Metasurface structures have proven to be effective in enhancing terahertz sensing signals and can thus be used as sensors to improve terahertz detection sensitivity. However, the sensitivity is limited by the poor spatial overlap between the analytes and the local electric field of the metasurface. In this work, a novel design of a floating bilayer metasurface structure for terahertz sensing is proposed and investigated. This structure supports a sharp toroidal dipole resonance and can concentrate near‐field energy on the analyte and metal atoms rather than on the substrate surface by floating the metal atoms. Consequently, the sensitivity is significantly improved to as high as 362 GHz RIU−1; theoretically, this is approximately 2.6 times higher than that of the common metasurface. The ability of the floating bilayer metasurface to quantitatively detect chlorothalonil is experimentally demonstrated. The resonance peak shows a significant frequency shift of 7 GHz for a change of 0.0001 mg dL−1 in chlorothalonil concentration, reaching up to 86 GHz when the change in chlorothalonil concentration is 100 mg dL−1; this is approximately 6.6 times higher than that of the common metasurface. This work provides opportunities for metasurface to realize ultrasensitive sensing in the terahertz regime.