Electronic devices capable of perceiving and responding to environmental changes are essential for applications in human–machine interaction, monitoring systems, and robotics. However, most existing devices struggle with the separation of sensing and actuation, resulting in complex integration and limited responsiveness. Here, inspired by the interplay between sensory and muscle cells in sea anemones, we present an intelligent thermoelectric device that seamlessly combines multimodal sensing with autonomous thermal actuation, achieving a closed-loop sensory-motor reflex. The device exhibits excellent temperature sensitivity (0.2 °C) and pressure resolution (0.03 mm), attributable to its three-dimensional (3D) architecture and hierarchical conductive network. Molecular dynamics simulations reveal that a dynamic hydrogen-bonding network enhances stress dissipation and interfacial adhesion, ensuring exceptional mechanical stability over 140,000 cycles. Notably, it also features thermal self-adaptation, actively triggering a protection mechanism to avoid high-temperature stimuli via thermoresponsive deformation, with an adjustable actuation threshold. This work advances intelligent electronics with real-time decision-making and environmental interaction.