Electron acceptor-initiated polymerization is as an effective approach to produce TSCT polymers with tunable aggregate emission by introducing various donor-type monomers or end groups. In light of the fact that charge transfer occurred between aromatic solvent molecules and PDI-tetraBr dependent on the electron density of the solvents (Figure , F and G), we anticipated that the introduction of polymeric donor matrix by PDI-tetraBr-initiated polymerization may facilitate the aggregate emission of PDI. We hypothesized that polymeric donor groups might effectively bind to the PDI scaffold via D-A charge transfer processes in the aggregate state, and this conformation could induce distortions on PDI co-facial π-π stacking, while expanding the distance between PDI scaffolds in a limited degree.