Mussel byssal threads are well-known due to their self-healing ability after the mechanical stress caused by waves. The proposed mechanism demonstrates the importance of reversible histidine-metal interactions as well as the block copolymer-like hierarchical architecture of the underlying protein structure. Taking these two aspects as inspiration for the design of synthetic analogs, different histidine-rich block copolymers were synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization. The hard domain was mimicked using polystyrene and the soft domain consists of n-butyl acrylate (BA) as well as histidine moieties as ligands. The block copolymers were crosslinked using different zinc(ii) salts and the resulting metallopolymers were investigated with respect to their self-healing abilities. The observed two-step mechanism of the self-healing process was studied in detail. Furthermore, the mechanical properties were determined by nanoindentation and were correlated with other results.