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Recently, a composite force sensor based on UCNPs embedded in a polystyrene microbead enabled the first real\u2010time measurement of feeding forces in living nematodes. However, the comparatively large stiffness of polystyrene only makes it relevant to biomedical applications in a small subset of biological tissue. To facilitate deployment of UCNPs into biological tissues with a range of mechanical properties, we expand upon polymer\u2010UCNP composite systems by embedding UCNPs in three polymer matrices with varying stiffnesses (epoxy resin, polydimethylsiloxane, and alginate hydrogels). Furthermore, to enhance these composites\u2019 mechanosensitivity, we methodically investigate using two different core\u2013shell architectures of SrLuF\u2010based UCNPs doped with ytterbium, erbium, and varying manganese concentrations. We calibrate polymer\u2010UCNP composite optical force sensitivity with colocalized atomic force and confocal microscopy. Using the red to green emission ratio (\u0394% I\n                    <jats:sub>Red<\/jats:sub>\n                    :I\n                    <jats:sub>Green<\/jats:sub>\n                    ) as the force read\u2010out, we determine that SrLuF:Yb\n                    <jats:sub>0.28<\/jats:sub>\n                    Er\n                    <jats:sub>0.025<\/jats:sub>\n                    Mn\n                    <jats:sub>0.013<\/jats:sub>\n                    @ SrYF dispersed in epoxy resin exhibits the greatest emission color change (12 \u0394%I\n                    <jats:sub>Red<\/jats:sub>\n                    :I\n                    <jats:sub>Green<\/jats:sub>\n                    per microNewton). Finally, we map forces in the epoxy\u2010UCNP composite on the macroscale between the joint of a chicken wing bone using a commercially available wide\u2010field microscope, thereby demonstrating its ability to optically measure pressures in situ. This work establishes the utility and modularity of the UCNP\u2010polymer composite system for force\u2010sensing in geometrically and mechanically diverse biological systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.202522706","type":"journal-article","created":{"date-parts":[[2026,4,20]],"date-time":"2026-04-20T13:47:34Z","timestamp":1776692854000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Mechanosensitive Polymer Matrices of Biologically\u2010Relevant Compliance Based on Upconverting Nanoparticles"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8461-156X","authenticated-orcid":false,"given":"Cindy H.","family":"Shi","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering Stanford University  Stanford California USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mia 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