Stretchable, flexible sensors are one of the most critical components of smart wearable electronics and Internet of Things (IoT), thereby attracting multipronged research interest in the last decades. Following miniaturization and multicomponent development of several sensors in one could further propel the demand for wireless, multimodal platforms. Greener substitutes to conventional sensors that can operate in a self-powered configuration are highly desirable in terms of all-in-one sensor utilities. However, fabrication of composite-based ultrastretchable, self-powered sensors with multifunctionality, robustness, and conformability is still only partially achieved and, therefore, demands further investigation. In this work, we report a triboelectric nanogenerator (TENG)-based multifunctional strain and organic vapor sensor using cross-linked ethylene propylene diene monomer (EPDM) elastomer and conducting carbon black as active fillers in the presence of an ionic liquid. The resulting piezoresistive sensor demonstrates ultrahigh gauge factor (GF > 220k) and wide range strain sensitivity and is, therefore, suitable for subtle-to-high frequency motion detection devices. Supported by excellent triboelectric outputs (force sensitivity 0.5 V/N in the range of 50–300 N, maximum output voltage VOC ∼ 178 V, short circuit current ISC ∼ 18 μA, maximum power density 0.11 mW/cm2), the hybrid sensors offer remarkable mechanical toughness and seamless voltage generation under contact-separation, even after several thousand cycles of operations. Furthermore, the sensor substrates exhibited reproducible organic vapor-sensing behavior, with high responsivity of 1.92 and 1 for ethanol and acetone, respectively, under flowing vapor conditions. This work lays a strong foundation for developing a truly multimodal, TENG-based, self-powered organic vapor and strain sensors.