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The surface morphology of viscoelastic-sensitive films significantly affects sensing characteristics of surface acoustic wave (SAW) sensors. Uniformity and compactness of the film surface directly influences detectability of the SAW sensor toward target gases. Viscoelastic fluoroalcoholpolysiloxane (SXFA) was prepared in this work using spin coating technology on an SAW delay line of 200 MHz and then used as coating for detection of dimethyl methylphosphonate (DMMP). Polarizing, atomic force, and scanning electron microscopies confirmed the uniformity of the SXFA surface. The particle diameter in the cluster region was 10-15 μm. The contact angle (5.72-26.69°), surface tension (21.053-29.155 mN/m), Gibbs free energy (-160.68 to -153.45 J/m 2 ), and spreading coefficient (0.3028-6.9453 J/m 2 ) of different concentrations of SXFA were obtained through experiments, and their relation was analyzed using the Young T equation and Gibbs adsorption isotherm. The glass transition temperature (-19.7 °C) and elasticity of SXFA were also discussed. The consistency of sensor preparation was confirmed by detecting DMMP with five SAW sensors prepared simultaneously. Seven consecutive tests showed that the SAW sensor presents satisfactory repeatability (standard deviation, s , 1.134; coefficient of variance, v , 0.065; and population mean deviation, δ, 0.913) at a concentration of 1.71 mg/m 3 and acceptable linear relationship at a concentration range of 0.058-1.92 mg/m 3 , with a sensitivity of around 1.21 mv/(mg/m 3 ). The sensor exhibited outstanding sensitivity and satisfactory linearity and repeatability to DMMP. Meanwhile, the sensing mechanism in gas adsorption was also discussed in terms of LSER formulation and hydrogen bonding formation between SXFA and DMMP.