In this chapter, we have briefly summarized aspects of supramolecular materials nanoarchitectonics using several examples, mainly from our recent accomplishments. Structural control over molecular arrays and materials arrays provides nanoscale structures, where molecular attributes such as morphology and functional group positioning require thoughtful design. For micro-sized objects obtained through self-assembly, careful design of component structures is indispensable for successful assembly. Intentional assembly such as LbL assembly is quite an effective means to construct highly desirable functional microstructures. Finally, some techniques such as dynamic manipulation of self-assembled molecules at the air-water interface can provide unique media for coupling of bulk mechanical motions with molecular function. These systems are mainly related to bottom-up processes in nanofabrication. Coupling of these exploratory researches with well-developed microlithography techniques will create meaningful and useful integrations of bottom-up and top-down nanotechnologies.