very desirable to extend their lifespan and be considered as materials derived from renewable resources. [4] The initial report on self-healing materials came from White et al. [5] They designed an encapsulating monomer that was released after cracks broke the capsule and then polymerized within the cracks after mixed with an initiator/catalyst embedded in the matrix.Currently, intrinsic self-healing polymers embedded with reversible dissociation of chemical bonds have become the mainstream of development and are widely used in the research of artificial skin, conductive elastomers, and soft robots. [6] Two approaches, typically, have been employed to construct such self-healing systems, one of which involves the use of noncovalent bonds. What has been widely studied is a macroscopic self-healing system using hydrogen bonding, [7] π-π stacking, [8] and hydrophobic interaction, [9] which includes high repeatability and reactivity of the repair reaction. The second approach relies on dynamic (reversible) covalent bonds, which mainly include systems based on reversible Diels-Alder reactions, [10] reversible reactions of imine moieties, [11] metal ion-ligand binding system, [4a] disulfide exchanges, and radical reshufflings of trithiocarbonates. [12] This self-healing system may potentially provide materials with higher stability and higher mechanical strength.The cross-linked structure is usually designed and embedded in the self-healing polymer system to retain their shape and to improve the mechanical strength of the material. [7a] So far, the main method reported to form cross-linked structures is to incorporate multifunctional reactive monomers into polymer systems [13] or to create metal ion-ligand coordination between molecular chains. [14] However, the employment of multifunctional reactive monomers or macromolecular segments so far usually results in difficult or incomplete degradation, which places a heavy burden on the natural environment, especially in marine ecosystems. [13,15] We conceive herein a design concept that uses the reversible bond of the imine part, the metal ion-imine ligand coordination, and the crystallites to jointly adjust the type and strength of the cross-linking structure to achieve cross-linking, high stretchability, self-healing, and complete degradability. Notably, previous work involving the metalligand interaction of self-healing materials either relied on the Environmentally friendly materials with good adjustable mechanical properties, modifiability, self-healing properties, and entirely degradable properties promote technological progress, but they fail to integrate all the attributes in a single platform. Herein, a design concept is conceived that uses the reversible bond of imine part, the metal ion-ligand coordination, and the crystallites to jointly adjust the internal structure of poly-Schiff base (PSB) metal complexes to achieve cross-linking, high stretchability, self-healing, and complete degradability. The metal ion-imine ligand coordination controls the degree ...