Integration of sensing and actuation capabilities into flexible electronics is critical to expanding their applications. Existing stimuli-responsive polymers fail to achieve satisfactory requirements, considering their strength− toughness trade-off, conductivity, and recyclability. Here, a novel stimuli-responsive elastomer is reported by molecular design, thus simultaneously enabling the effective unification of sensing and actuation functions. The stimuli-responsive elastomer realizes high strength (32 MPa), high stretchability (527%), high toughness (74.8 MJ• m −3 ), high fracture energy (75,300 J•m −2 ), efficient recyclability processability, puncture-resistance, and high conductivity (120.1 S•m −1 ) where the conductive elastomer is created by incorporating both dynamic covalent bonds (strong bonds)/ coordination bonds (weak bonds) for the formation of dynamic adaptive networks and coated conductive ink. In parallel, benefiting from the sensing actuation mechanism from its architecture, the elastomer-enabled sensor and actuator achieve both exceptional sensing performance as a green strain sensor for monitoring body movements and excellent actuation ability as a green self-sensing actuator for load-carrying. Overall, this comprehensive elastomer brings new inspiration and insights into the design of next-generation green e-skin, flexible robots, and other stimuli-responsive materials.