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Herein, inspired by the dynamic architecture of living systems, the construction of \u201cliving\u201d biodegradable hydrogel microspheres is reported that reconcile this contradiction through internal nano\u2010reinforcement and external molecular lubrication. Crystalline disc\u2010like Laponite nanosheets are intercalated within GelMA networks, acting as dynamic, spatially confining crosslinkers that inhibit water infiltration and preserve network cohesion. Concurrently, zwitterionic brushes are grafted onto the microsphere surface, forming a robust hydration layer via dynamic charge\u2013dipole interactions to enable long\u2010lasting lubrication. This synergistic design endows the microspheres with tunable elasticity (14\u20134000\u00a0Pa) and adjustable friction coefficients (0.12\u20130.04), achieving a functional convergence of mechanical resilience and surface lubricity. Experimental evaluations confirm their efficacy in inhibiting excessive mechanical stress\u2010induced calcium ion influx and downstream calcium signaling to prevent chondrocyte damage. This work offers a universal strategy to overcome the elasticity\u2013lubrication paradox in hydrogels, unlocking their potential in biomedical engineering, drug delivery, and soft robotic interfaces.<\/jats:p>","DOI":"10.1002\/smll.202507138","type":"journal-article","created":{"date-parts":[[2025,9,18]],"date-time":"2025-09-18T11:45:56Z","timestamp":1758195956000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Nano\u2010Confined Hydrogel Microspheres with Programmable Mechanics and Molecular Lubricity"],"prefix":"10.1002","volume":"21","author":[{"given":"XiaoXiao","family":"Li","sequence":"first","affiliation":[{"name":"Department of Orthopaedics Center for Spinal Minimally Invasive Research Shanghai Key Laboratory of Flexible Medical Robotics Institute of Medical Robotics Tongren Hospital Shanghai Jiao Tong University School of Medicine  Shanghai 200336 P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiangyang","family":"Xu","sequence":"additional","affiliation":[{"name":"Department of Orthopaedics Shanghai Key Laboratory for Prevention and Treatment of Bone and Joint Diseases Shanghai Institute of Traumatology and Orthopaedics Ruijin Hospital Shanghai Jiao Tong University School of Medicine  197 Ruijin 2nd Road Shanghai 200025 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6938-9582","authenticated-orcid":false,"given":"Wenguo","family":"Cui","sequence":"additional","affiliation":[{"name":"Department of Orthopaedics Shanghai Key Laboratory for Prevention and Treatment of Bone and Joint Diseases Shanghai Institute of Traumatology and Orthopaedics Ruijin Hospital Shanghai Jiao Tong University School of Medicine  197 Ruijin 2nd Road Shanghai 200025 P. R. 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