Precise control of epitaxial growth of MOF-on-MOF thin films, for ordered hierarchical tbo-type structures is demonstrated. The heterostructured MOF thin film was fabricated by successful sequential deposition of layers from two different MOFs. The 2-periodic layers, edge-transitive 4,4-square lattices regarded as supermolecular building layers, were commendably cross-linked using a combination of inorganic/organic and organic pillars.