The behavior of asphalt mixtures is very complicated due to structural configuration and interfacial friction of aggregates as well as chemical and rheological reactions of the asphalt binder itself or with the aggregates. Furthermore, this complex response is more complicated under various loads, temperatures, and other environmental factors. To control the complex responses and reduce the complex factors, a DSR moisture damage test using small rock disks was developed. This paper focuses on the more fundamental concepts to explain asphalt and asphalt–aggregate bond behavior exhibited under the newly-developed DSR moisture damage test. The traditional model of asphalt structure is based on the theory of colloid and surface chemistry. Although this traditional model can explain many physical phenomena of asphalt structure, it cannot explain all the asphalt behaviors, such as steric hardening. Therefore, more general, but fundamental concepts may be required to attain insight of the material. As one of the possible concepts, a self-assembly concept in supramolecular chemistry is proposed and phenomena and results of the DSR moisture damage test are explained by the concept.