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Electroadhesion provides a promising route to augment robotic functionalities with continuous, astrictive, and reversible adhesion force. However, the lack of suitable conductive/dielectric materials and processing capabilities have impeded the integration of electroadhesive modules into soft robots requiring both mechanical compliance and robustness. We present herein a novel iontronic adhesive based on a dynamically crosslinked gel-elastomer system, including an ionic organohydrogel as adhesive electrodes and a resilient polyurethane with high electrostatic energy density as dielectric layers. Through supramolecular design and synthesis, the dual-material system exhibits cohesive heterolayer bonding and autonomous self-healing from damages. Iontronic soft grippers that seamlessly integrate actuation, adhesive prehension, and exteroceptive sensation are devised via additive manufacturing. The grippers can capture soft and deformable items, bear extreme payload under reduced voltage input, and rapidly release foreign objects in contrast to electroadhesives. Raw data of materials characterization and devices testing are deposited here.