Strong, Smart, and Slippery Organo‐gels by Network Glassification

Abstract Lubricant‐infused organo‐gels with low surface energy solvents represent an environment‐friendly lubricating material, while the poor mechanical performance incapacitates them to harsh and intricate service conditions. To address this challenge, a simple yet highly effective strategy to prepare strong, smart, and slippery organo‐gels by glassifying the polymer network is reported. As a proof of concept, appropriate amounts of rigid solvophobic poly(phenyl methacrylate) (PPMA) units are integrated into a solvophilic poly(cyclohexyl acrylate) (PCHA) network infiltrated with lubricant. Upon forming bicontinuous phase‐separated structures, the rigid solvent‐free PPMA segments stay in glassy states, serving as a load‐bearing phase to toughen the materials effectively. Meanwhile, the soft PCHA phase maintains lubricity and extensibility by holding a substantial amount of lubricant. Owing to the synergistic effect, the gels manifest glass‐like mechanical performance with high rigidity (46.6 MPa), strength (7.7 MPa), and toughness (23.7 kJ m⁻²). Moreover, the materials exhibit high thermo‐sensitivity with the elastic modulus reversibly decreasing from 46.6 MPa at 20 °C to 0.23 MPa at 50 °C, endowing the gels with shape‐memory properties. Furthermore, the organo‐gels display satisfactory anti‐adhesiveness to various foreign matters. Taken together, the work represents a facile and universal strategy to reinforce organo‐gels, thereby adapting them to various applications.