A strategy for SERS-based ultrasensitive detection of sarin-simulant is presented. Surface-modified SERS substrate can preferentially capture the sarin-simulant agent. Raman peak intensity shows a linear double logarithmic relation with simulant content. Such linear relation arises from Freundlich adsorption of simulant on the substrate. The limit of detection for sarin-simulant agent is down to about 1 ppb.