Hyperelastic materials exhibit a nonlinear elastic response to large strains, whereas hydrogels typically possess a low elastic range due to the nonuniform cross-linking and limited chain segments among cross-links. We developed a hyperelastic hydrogel that possesses a broader elastic range by introducing a reversible pearl-necklace structure, in which beads are connected by strings. The subnanometric beads can efficiently unfold and refold under cyclic mechanical strains; thus, the hydrogel can rapidly recover after being stretched to an areal strain of more than 10,000%. Additionally, the hydrogel can quickly heal from minor mechanical damages such as needle punctures and cuts. These advancements make our ionic hydrogels ideal for multifunctional pneumatic gripper materials; they simultaneously offer an ultralarge gripping range, self-sensing capabilities, and fast healing abilities.