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Lanthanide‐based upconverting nanoparticles (UCNPs) are largely sought‐after for biomedical applications ranging from bioimaging to therapy. A straightforward strategy is proposed here using the naturally sourced polymer phytoglycogen to coencapsulate UCNPs with hydrophobic photosensitizers as an optical imaging platform and light‐induced therapeutic agents. The resulting multifunctional sub‐micrometer‐sized...