Perching-and-takeoff robot can effectively economize onboard power and achieve long endurance. However, dynamic perching on moving targets for a perching-and-takeoff robot is still challenging due to less autonomy to dynamically land, tremendous impact during landing, and weak contact adaptability to perching surfaces. Here, a self-sensing, impact-resistant, and contact-adaptable perching-and-takeoff robot based on all-in-one electrically active smart adhesives is proposed to reversibly perch on moving/static dry/wet surfaces and economize onboard energy. Thereinto, attachment structures with discrete pillars have contact adaptability on different dry/wet surfaces, stable adhesion, and anti-rebound; sandwich-like artificial muscles lower weight, enhance damping, simplify control, and achieve fast adhesion switching (on-off ratio approaching
∞
in several seconds); and the flexible pressure (0.204% per kilopascal)–and–deformation (force resolution, <2.5 millinewton) sensor enables the robot’s autonomy. Thus, the perching-and-takeoff robot equipped with electrically active smart adhesives exhibits tremendous advantages of soft materials over their rigid counterparts and promising application prospect of dynamic perching on moving targets.