Rapid and reversible actuation and shape memory effects are critical for biomimetic soft actuators based on polymer hydrogels. However, most conventional hydrogel actuators show very slow actuation or deformation rates in water. It remains a challenge to realize rapid actuations, particularly for hydrogels to actuate in air. Here, a novel strategy to create diverse hydrogel devices with shape memory effects and rapid reversible actuations even in air was demonstrated. This strategy relies on a precise definition of local crosslinking by using multivalent metal ion coordination. This is demonstrated by infiltrating Fe³⁺ ions into stretchable nanocomposite polyacrylamide hydrogels with the amide groups converted into primary amine groups for multivalent coordination and crosslinking. The Fe³⁺ coordination with amine groups enhanced the crosslink density and modulus, leading to deswelling. By using an iron rod electrode, the Fe³⁺ coordination and crosslinking were precisely controlled to generate hydrogels with heterogeneous local crosslinking, including Janus hydrogels, S-shaped hydrogels, and cross-shaped hydrogel grippers. These soft devices were reversibly actuated in tens of seconds when cyclically dehydrated in ethanol and rehydrated in water. Most interestingly, very rapid reversible actuations of a hydrogel device in air were demonstrated by using electro-redox reaction of Fe³⁺ and Fe²⁺ in the hydrogel, where the reversible local coordination crosslinking and decomposition served as a hinge to actuate the hydrogel. This strategy based on reversible local coordination and crosslinking may open an avenue for rapid fabrication of hydrogel devices with well-defined structures and actuation properties.