Smart environments, integrating different sensors and other technology solutions, are one of the key direction in which everyday spaces in buildings are expected to develop in the future. One aspect of smart environments includes large interactive surface areas, which are embedded to walls, tables or other furniture. This chapter introduces how service design methods have been applied in our research on smart surfaces, and discusses different design methods and their strengths in this context. Specifically, we present three service design cases, interactive wallpaper, a smart building infrastructure and a smart cafe table, and how the related use cases have been studied with service design methods. These three design cases are positioned at different maturity levels of the product development process, the interactive wallpaper and smart building representing early design concepts, and the interactive table a functional prototype.