Here, we demonstrate a bottom-up approach for the fabrication of well-defined dimensional-crossover nano-architectures with high tunability using metals and organic molecules as building blocks or linkers. We succeeded in rationally constructing assemblies; (1) ladders and tubes which are located in dimensional-crossover region between 1D and 2D, (2) surface metal–organic frameworks (SurMOFs) which are located in dimensional-crossover region between 2D and 3D, and (3) nanoparticles coated with MOFs or polymers which are located in dimensional-crossover region between 0D and 3D.