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Aqueous surface gels are fragile yet resilient biopolymer-based networks capable of sustaining extremely low friction coefficients despite tribologically-challenging environments. These superficial networks are ubiquitous in natural sliding interfaces and protect mechanosensitive cells from excessive contact pressures and frictional shear stresses from cell-fluid, cell-cell, or cell-solid interactions. Understanding these complex lubrication mechanisms may aid in the development of materials-based strategies for increasing biocompatibility in medical devices and implants. Equally as important is characterizing the interplay between soft and passive yet mobile implant materials and cellular reactions in response to direct contact and frictional shear stresses. Physically interrogating living biological systems without rupturing them in the process is nontrivial. To this end, custom biotribometers have been designed to precisely modulate contact pressures against living human telomerase-immortalized corneal epithelial (hTCEpi) cell layers using soft polyacrylamide membrane probes. Reverse-transcription quantitative polymerase chain-reaction (RT-qPCR) indicated that increased duration and, to a much greater extent, the magnitude of frictional shear stress lead to increased production of pro-inflammatory (IL-1β, IL-6, MMP9) and pro-apoptotic (DDIT3, FAS) genes, which in clinical studies are linked to pathological pain. The hierarchical structure often found in biological systems has also been investigated through the fabrication of high-water content (polyacrylamide) hydrogels through free-radical polymerization inhibition. Nanoindentation experiments and friction coefficient measurements indicate that these "gradient surface gels" reduce contact pressures and frictional shear stresses at the surface of the material while still maintaining stiffness within the bulk. Reducing frictional shear stresses through informed materials and surface design may concomitantly increase lubricity and quiet the immune response, and thus provide bio-inspired routes to improve patient outcomes and quality of life.