Terpyridine-polyethyleneglycol-block-polyleucine block copolymer (tpy-PEG-PLeu) was synthesized by a ring-opening polymerization of L-leucine -carboxyanhydride. The copolymer complexed with ion and its aqueous solution showed a purple color as a result of the complexation. This complexation caused the diblock/triblock structural transition of the copolymer. The change of the aggregation behavior caused by the structural transition was observed by a dynamic light scattering apparatus. The diblock tpy-PEG-PLeu copolymer formed a micelle in the aqueous solution. On the other hand, the triblock-type copolymer, after the complexation, formed the micelle structures and huge aggregates, which is considered to be a network structure. The complexation of the diblock tpy-PEG-PLeu copolymer with Fe ion is consequently considered to be a trigger of the gelation.