Molecular self-assembly based on coordination chemistry has made an explosive development in recent years. Over the last >30 years, we have been showing that the simple combination of transition-metal’s geometry (typically, a 90 degree coordination angle of Pd(II) center) with organic bridging ligands gives rise to the quantitative self-assembly of nano-sized, discrete organic frameworks. Representative examples include square molecules (1990), linked-ring molecules (1994), cages (1995), capsules (1999), and tubes (2004) that are self-assembled from simple and small components. Originated from these earlier works, current interests in our group focus on i) molecular confinement effects in coordination cages, ii) solution chemistry in crystalline porous complexes (as applied to “crystalline sponge method”), and iii) and giant self-assemblies, as disclosed in this lecture.