For materials development with high-level structural regulations, the emerging concept of nanoarchitectonics has been proposed. Analytical sciences, including sensing/detection, sensors, and related device construction, are active targets of the nanoarchitectonics approach. This review article focuses on the two features of interface and nanostructures are especially focused to discuss nanoarchitectonics for analytical science. Especially, two selected topics, (i) analyses on molecular sensing at interfaces and (ii) sensors using self-assembled supramolecular nanostructures, are exemplified in this review article. In addition to recent general examples, specific molecular recognition at the air-water interface and fabrication of sensing materials upon self-assembly of fullerene units are discussed. Descriptions of these examples indicate that nanoarchitectonics and analytical science share common benefits, and therefore, developments in both research fields should lead to synergies.