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Polychaete worms display a remarkable jaw structure, where a gradient in metal-ligand coordination down thelength of the jaw results in a shift from hard to soft mechanics. To mimic these gradient structures, a Zn-coordinated supramolecular polymer is crosslinked into a covalent matrix to afford supramolecular semi-in-terpenetrating networks (SIPNs). These SIPN materials exhibit improved mechanics with a lower supramolecularcontent (30 wt%), allowing for energy dissipation through cavitation to increase material toughness. The shift inmechanical behavior is further attributed to the morphology, where the size of the phase-separated droplets andnature of the continuous phase in these SIPNs contributes to the material mechanics. Furthermore, chemicalgradients are applied to these systems through exposure to a competitive ligand, offering control over the lo-calization of supramolecular interactions. These materials offer a framework to mediate mechanics whilemaintaining the ability to program gradient supramolecular interactions.