<p>The dual-crosslinking strategy, in which both reversible dynamic crosslinks and robust static crosslinks are introduced into a polymer network, has emerged as a powerful method for enabling a combination of mechanical robustness and dynamic functions such as energy dissipation in a single elastomer. However, the contribution of dynamic crosslinks to overall mechanical performance, especially the roles of their thermodynamic and kinetic properties, remains insufficiently understood. To address this challenge, we introduced static crosslinks and various types of dynamic crosslinks into a model dual-crosslinked elastomer system. This network incorporates both covalent crosslinks and dynamic metal‒ligand coordination complexes that are distinct in their thermodynamic and kinetic properties. The thermodynamic and kinetic parameters of the corresponding metal–ligand complexes were quantified through model small-molecule studies using solution ultraviolet–visible (UV‒Vis) spectroscopy. The mechanical performance of the dual-crosslinked elastomers was strongly correlated with the dissociation constants of the metal‒ligand crosslinks. Specifically, faster bond dissociation led to accelerated stress relaxation and increased energy dissipation but at the expense of reduced toughness. These findings will pave the way for rationally engineering the mechanical properties of elastomers through the selection of dynamic crosslinks.</p>