Dynamic Network Reconfiguration Toward Mechanically Robust Polymeric Foam via Ice Templating

Polymeric foams have garnered significant interest in advanced engineering applications due to their unique porous architectures. Ice templating represents a promising strategy for creating polymeric foams with tunable pore morphology, yet faces practical constraints including reliance on energy‐intensive lyophilization and/or insufficient mechanical properties of the resulting foams. To address this challenge, a strategy is developed to prepare mechanically robust polymeric foams by photo‐crosslinking ice‐templated emulsions. By incorporating dynamic hindered urea bonds into the emulsion, dynamic network reconfiguration is achieved, which dramatically improves mechanical properties. The resultant foam (≈65% porosity) exhibits tensile strength and breaking strains of 7.9 MPa and 533%, with toughness of 15.8 MJ m −3 . In addition, this strategy permits the construction of intricate 3D architectures using 3D‐printed sacrificial thermoplastic templates, expanding their potential applications in demanding engineering scenarios.