The preparation of crystalline, ordered thin films of metal–organic frameworks (MOFs) will be a critical process for MOF-based nanodevices in the future. MOF thin films with perfect orientation and excellent crystallinity were formed with novel nanosheet-structured components, Cu–TCPP TCPP = 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin, by a new “modular assembly” strategy. The modular assembly process involves two steps: a “modularization” step is used to synthesize highly crystalline “modules” with a nanosized structure that can be conveniently assembled into a thin film in the following “assembly” step. With this method, MOF thin films can easily be set up on different substrates at very high speed with controllable thickness. This new approach also enabled us to prepare highly oriented crystalline thin films of MOFs that cannot be prepared in thin-film form by traditional techniques.