This paper presents a new effective approach for the sensitive film deposition of surface acoustic wave (SAW) chemical sensors for detecting organophosphorus compounds such as O-ethyl-S-2-diisopropylaminoethyl methylphosphonothiolate (VX) containing sulfur at extremely low concentrations. To improve the adsorptive efficiency, a two-step technology is proposed for the sensitive film preparation on the SAW delay line utilizing gold electrodes. First, mono[6-deoxy-6-[(mercaptodecamethylene)thio]]-β-cyclodextrin is chosen as the sensitive material for VX detection, and a ~2 nm-thick monolayer is formed on the SAW delay line by the binding of Au-S. This material is then analyzed by atomic force microscopy (AFM). Second, the VX molecule is used as the template for molecular imprinting. The template is then removed by washing the delay line with ethanol and distilled water, thereby producing the sensitive and selective material for VX detection. The performance of the developed SAW sensor is evaluated, and results show high sensitivity, low detection limit, and good linearity within the VX concentration of 0.15-5.8 mg/m3. The possible interactions between the film and VX are further discussed.