Abstract Dynameric solid films may be generated via the adequate imine‐bond connection between bis(pyridine‐2,6‐diimine) core centres, coordinated with different metal cations and diaminoPEG connectors. The adequate selection of metal cations leads to cross‐linked metallo‐dynameric films, allowing the fine modulation of their colour and mechanical property. The coordination of the metal cations and bis(pyridine‐2,6‐diimine), results in the formation of interlocked structures, leading to the most probably formation of interweaved structures with better mechanical properties than those formed in the absence of the metallic cations. Removal and addition of metal cations from solid films can be achieved via tris(2‐aminoethyl)amine (TREN) complexing agent, which strongly binds the metal cations, followed by subsequent insertion of other metallic cations. It allows a ligand‐modulated dynamic release of the metal cations from the solid films, together with colour transfer and change of mechanical strength at the interfaces between various solid films.