Smart Systems collate leading technologies and solutions for the design of new generation embedded and cyber-physical systems. They can be applied to a broad range of application domains, from everyday life to mission and safety critical tasks, and achieve a wide set of functionality using diverging architectures. Smart system design needs to be achieved in a real multi-domain environment, where analog, digital, mixed-signal, and now even MEMS sub-systems tightly interact. With a traditional approach, these different units are designed separately, and finally merged at the electronic system level. However, given the increasing integration and interactions among components of different nature, methodologies enabling effective system-level architectural exploration are becoming more and more significant. Starting from a detailed analysis and classification of state-of-the-art use scenarios, and based on a review of the existing approaches, we present a top-down constraint-driven methodology for the design of new generation smart systems. It enables partitioning and propagation of high-level application-driven requisites towards low-level units in the design flow. The methodology reviews fundamental and cross-sectional system-level design aspects applied to the definition of an example case, to identify sub-system requirements towards the specifications of the electrical features of each internal unit.