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.
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