Reinforcement of the covalent network with PEC self-assemblies improved the tensile performance of GelMA hydrogels. Stress-strain curves from uniaxial tensile tests (Figure , S11) revealed significant enhancements in ultimate stress (up to 572%, Figure ), extensibility (up to 42%, Figure ), Young's modulus (up to 1147%, Figure ), and toughness (up to 772%, Figure ) for photocrosslinked GelMA/bPE hydrogels. In these hybrid hydrogels, the selfassembled bPEs served as energy-dissipating scaffolds within the brittle GelMA network. Due to the reversible nature of electrostatic interactions, the PEC domains were hypothesized to undergo repeated sequences of disassembly and reassembly without influencing the integrity of the GelMA network. Higher bPE loading enhanced the overall network resilience, requiring higher energy to break the network.