Markedly Strengthened Delayed Fluorescence and Processability in Crystalline Hybrids via Solvation-Enhanced Self-Dissolution–Recrystallization

Crystalline afterglow materials hold broad application potential yet suffer from poor processability. Herein, we report a strategy that enhances both processability and luminescence through solvation-enhanced self-dissolution–recrystallization. Two low-cost, nonaromatic inorganic–organic afterglow hybrids─featuring solvated Zn2+ ions─were prepared. Host–guest doping enables wide-range tuning of room-temperature phosphorescence (RTP) color and extended lifetimes. Thermal annealing further enhances RTP and strongly activates delayed fluorescence (DF), increasing the DF lifetime by up to 254×. This enhancement is driven by dehydration of Zn2+ and coordination to guest carboxylate groups, which suppresses nonradiative decay and promotes reverse intersystem crossing. Remarkably, abundant lattice water enables self-dissolution upon heating, recrystallization upon cooling, and full recovery via water vapor fumigation─conferring excellent processability. This work provides a new design route to low-cost, processable crystalline materials with multimodal and tunable long-lived luminescence.