This work extends recent developments in diacetylene-based, sprayable sensors by identification and assessment of formulations which facilitate their use for wearable sensing. Diacetylene-based spray-on sensors have the potential to be a widely deployed sensing technology, as they require no power and can be applied as thin coatings onto surfaces to provide a colorimetric response to target exposure. In responding to radiation, liquid-phase targets, or gas-phase targets specifically determined by the formulation of the sprayable sensor used, this technology is amenable to wearable sensors for measuring exposure to different environmental risks. Here, we provide the means to improve wear resistance, reduce false-positive signals due to wetting, and enhance color fastness for coatings of sprayable, diacetylene-based sensor formulations on cotton fabric. These sensor formulations possess polymethyl methacrylate (PMMA), which enhances the coating stability to only 8% color loss due to wear compared to 18–25% without PMMA, while maintaining the inherent ability of diacetylene-component formulations to detect radiation as well as gas or liquid phase analytes. This represents a significant step toward the use of diacetylene-based sensing formulations for wearable sensing. In the future, the form of spray-on sensor materials demonstrated here may find use in wearable sensing applications for detection of cumulative exposure to UV radiation, hydrogen peroxide vapors, or solvent exposure. We expect trends toward applications toward other wearable sensors for environmental monitoring given the well-known customizability in target response of diacetylene-containing monomers by modifying their headgroup chemistry.