Hydrogel networks formed via dynamic metal-coordination chemistry exhibit remarkable mechanical properties, such as self-assembly, stimuli-responsiveness, and the ability to self-heal, due to the dynamic and reversible nature of the metal-ligand interaction. Recent efforts have been directed at expanding the prevailing knowledge of metal ion-coordination chemistry to nanoparticle-ligand interactions, with the goal to further provide rational control over the mechanical properties of the gel. Although studies have focused on varying nanoparticle size, shape and type, little work has been conducted to understand how changing the functional group of the polymers affects the macroscopic mechanical properties of the hydrogel. Thus, this work explores the manipulation of crosslinking kinetics through ligand choice and its effect on the hierarchical control of hydrogel dynamics, and offers further guide in the rational design of gels for advanced engineering applications.