Constructing flexible ultralong room-temperature phosphorescence (URTP) materials is highly attractive yet challenging, as flexible matrices struggle to suppress the nonradiative decay of triplet excitons. Herein, self-protective carbonized polymer dots (CPDs) derived from carbonized polyvinyl alcohol (PVA), were embedded in a gel matrix to create flexible URTP materials. Simply tuning the alcoholysis degree of PVA to 88% and reacting it with ethylenediamine under hydrothermal conditions yields NCD88, which exhibits a phosphorescence lifetime of 1.05 s. This benefits from carbonyl/nitrogen clusters that promote intersystem crossing (ISC) and incompletely carbonized PVA chains that restrain nonradiative decay. This strategy effectively resolves the trade-off between ISC efficiency and triplet exciton stabilization, enabling URTP in PVA-based CPDs. Furthermore, by combining freeze–thaw cycling with a solvent exchange strategy, a PVA-based deep eutectic gel was prepared, exhibiting a URTP lifetime of 0.86 s, along with high tensile strength and high toughness. Thus, this study not only resolves the challenge of nonradiative decay in PVA-based self-protective CPDs via simple alcoholysis regulation, but also successfully integrates URTP properties with high mechanical performance into a single gel system, providing a new strategy for developing flexible URTP materials.
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