Conventional lubricating hydrogels struggle to simultaneously achieve excellent mechanical strength and interfacial lubrication due to the bulk and surface homogeneity. To address this, we developed a hydrogel with superior lubrication and load-bearing performance by selectively breaking bicontinuous microphase confinement on the hydrogel surface, in which the hydrogen-bond association within the microphase is dissociated to release the confined polymer chains. The bicontinuous matrix acts as the load-bearing phase, utilizing its percolated hydrophilic/hydrophobic microphase interfaces for dissipation (elastic modulus ∼417 MPa). The broken microphases form a brush-like lubricating layer with strong hydration and entropic repulsion (coefficient of friction ∼0.0029). This structure effectively reduces shear stress and blunts friction cracks to improve wear resistance, and the percolated hydrophilic phase maintains sustainable lubrication via self-regeneration (coefficient of friction ∼0.0034, 50 N load, 100k cycles). This system also exhibits a closed-loop recycling, retaining 98.5% of its friction-reducing capabilities even after 100 cycles of reuse. Among reported lubricating hydrogels, this system achieves the lowest coefficient of friction with the highest modulus. This strategy provides a sustainable, innovative solution for lubrication systems under extreme conditions.
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