The new and distinct surfaces provide an opportunity for the development of efficient atomically/molecularly-organized catalysts. The key factors of regulation and design of catalyst surfaces are structure, composition, oxidation state, distribution, morphology, polarity, etc. which should be organized at the surfaces. In the development of novel catalyst surfaces, new concepts and strategies regarding composition or structure are conceived, where in situ characterizations by surface science are inevitably important for understanding the origin and mechanism of the tremendous catalysis of surfaces. These key issues can be derived from single crystal surfaces and designed surfaces experimentally and theoretically.