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Growing evidence supports a critical role of metal-coordination complex crosslinking in soft biological material properties such as underwater adhesion and self-healing. Given their exploitation in such desirable material applications in nature, bio-inspired metal-coordinate complex crosslinking no doubt provides unique possibilities to further advance synthetic polymer materials engineering. Using bio-inspired metal-binding polymers, initial efforts to mimic these material properties have shown promise. In addition, novel opportunities for new fundamental insights on how hierarchical polymer network mechanics can be strongly coupled to supramolecular crosslink dynamics are also emerging. Early lessons from studies of these hierarchical chemo-mechanical couplings will be presented.