Manipulation of the properties of aggregation-induced emission luminogens (AIEgens) by combining self-assembling motifs has attracted significant interest as a promising approach to developing various advanced materials. In this study, pendant diphenylalanine–tetraphenylethylene (TPE) copolymers exhibiting the ability for self-assembly and AIE properties were synthesized via reversible addition–fragmentation chain-transfer (RAFT) copolymerization. The resulting anionic and non-ionic amphiphilic copolymers with a carbon–carbon main chain bearing diphenylalanine–TPE through-space interactions self-assembled into nanorods and nanofibers, showing blue emissions originating from the aggregation of TPE side chains in the assembled structures. Suitable tuning of the comonomer composition, monomer structure, and environmental conditions (e.g., solvent polarity) enables manipulation of the self-assembled structures, AIE properties, and aggregation-induced circular dichroism by achiral TPE units via through-space interactions with diphenylalanine moieties.