Recently, numerous mechanically robust synthetic hydrogels have been created. However, unlike natural loading-bearing materials such as cartilages and muscles, most hydrogels have inherently contradictory requirements, obstructing the design of hydrogels with characteristics of robustness and rapid self-recoverability. Herein, we present a facile strategy for constructing mechanically robust and rapidly self-recoverable hydrogels. The linear poly(acrylamide-co-itaconic acid) chains crosslink via coordination bonds and minimal chemical crosslinkers to form the hydrogel network. Such design endows the coordination interactions to be asymmetrically distributed. Under deformation, the coordination interactions exhibit a reversible dissociation-and-reorganization property, demonstrating a new mechanism for energy dissipation and stress redistribution. Thus, the hydrogels possess tensile strength up to 12.5 MPa and toughness up to 28.2 MJ/m3. Moreover, the inherent dynamic nature of the coordination bonds imparts these hydrogels with stretch rate- and temperature-dependent mechanical behavior as well as excellent self-recovery performance. The method employed in this study is universal and is applicable to other polymers with load-bearing yet rapid recovery conditions. This study will facilitate diverse applications of most metallosupramolecular hydrogels.