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The presented results show that intramolecular photon upconversion is a versatile concept for the development of highly efficient solid-state photon upconversion materials.The ability to modulate the adhesion of soft materials on-demand is desired for broad applications ranging from tissue repair to soft robotics. Research effort has been focused on the chemistry and architecture of interfaces, leaving the mechanics of soft adhesives overlooked. Stimuli-responsive mechanisms of smart hydrogels could be leveraged for achieving stimuli-re