Different block copolymers containing terpyridine were synthesized applying the reversible addition-fragmentation chain transfer (RAFT) polymerization. The block copolymers contain polystyrene as hard block, and the soft block consists of n-butyl acrylate (BA) as well as terpyridine units as ligand. These block copolymers were further cross-linked with several metal salts in order to tune the self-healing behavior. Metallopolymers cross-linked with manganese(II) chloride featured the best self-healing behavior. Furthermore, a two-step mechanism behind the self-healing process of these metallopolymers could be attributed to each block of the copolymer and was studied extensively. In addition, rheological parameters were determined and correlated with the other results.