Dynamic bonds have attracted growing interests from material researchers as they offer a variety of advanced properties, like shape memory, self-healing, recyclability, tuned relaxation, high toughness, surface adaptation, and so on. They also enable material to respond to external stimuli like heat, pH, light, humidity, electric fields, and magnetic fields. Within a wide range of different dynamic bonds, ionic interactions and metal-ligand coordinating bonds are of particular interest, as they can be found in many biomaterials, unlocking the potential to develop biomimetic and biocompatible materials. This dissertation reveals how ionic bonds affect mechanical properties of polymer materials including stiffness, stretchability, deformation recovery, strain rate sensitivity, and self-healing property. Moving on, the effect of including counterions in semi-interpenetrating hydrogels with polyelectrolytes is also studied. Based on the result, regulation of hydrogel stiffness with an electric field is realized. Finally, non-destructive methods of reclaiming polydimethylsiloxane (PDMS) crosslinked by metal-ligand coordinating bonds are tested. This dissertation starts with an investigation of how ionic interactions in elastomers affect their mechanical properties, specifically when the material is highly stretchable. This is realized by designing and making materials assembled from oppositely charged acrylic copolymers. we confirmed the formations of ionic bonds within the material via vibration spectroscopy techniques, and demonstrated through various mechanical test methods that ionic interactions can enhance stiffness, strength, and deformation recovery of materials, yet they also restrict stretchability. We also showed the strain rate sensitivity of these materials, and how hydrophilicity of material affects the self-healing property. Moving on from understanding the impact of ionic bonds on mechanical properties, we designed a semi-interpenetrating polymer network hydrogel containing polyelectrolyte complexes as well as counterions and its stiffness can be regulated with an electric field with minimal actuation. We showed that removing counterions by diffusion can increase the stiffness of the hydrogel. With this finding, we confirmed counterion removal via electrodialysis and realized reversible time-dependent stiffness control when applying an electric field. A model was implemented to simulate ion transport in the material. Finally, we designed a device in combination with the hydrogel which gives a spatially variable stiffness haptic interface controlled with an electric field and it has both reversibility and cyclability. In the final chapter, we focus on studying the dissolution kinetics of metal-ligand coordinated PDMS network. We confirmed removal of metal ions with tetrasodium ethylenediaminetetraacetic acid (EDTA·4Na) by comparing Fourier transform infrared (FTIR) spectra and monotonic tensile test results of material formed from original PDMS and reclaimed PDMS. Based on this finding, a network dissolution method was designed to measure dissolution kinetics of the material in EDTA·4Na solution. Impact of counterions, metal ions, and molecular weight on this process was demonstrated. The systematic study of polymers with dynamic bonds (ionic interactions and metal-ligand coordinating bonds) in this dissertation provides insights into the design of new advanced materials with various functionalities.