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The elimination of traditional thermal generators and the increase of renewable energy source access reduced the inertia of the power system, and thermostatically controlled loads have the potential to provide ancillary services to the power system. This paper introduces a decentralized control strategy for thermostatically controlled loads (TCLs), which focuses on assisting large-scale TCLs in providing frequency support to power systems while considering energy efficiency ratio and measurement error correction. Initially, the nonlinear relationship between heat flow and TCLs’ power is modeled using a polynomial relationship, and the coefficients are determined through a data-driven method to enhance accuracy in TCLs modeling and assess their regulation potential precisely. Subsequently, a decentralized control strategy tailored for power system frequency regulation is developed. To account for measurement errors in TCLs controllers, a measurement error back-correction method is proposed. Simulation examples demonstrate the effectiveness of the proposed control strategy in achieving accurate modeling and control of TCLs and reducing power system frequency fluctuations.