The issue of sustainability of smart cities is approached in this chapter from two different angles: dimensions sector-specific and city governance. Following a short review of smart city sectors, emphasis is placed on the concept of smart governance of cities. The concept of smart governance is reviewed especially regarding cooperation with city governments of other cities within the region or country and empowering citizens. Different levels are presented with focus on four main conditions for smart governance, namely participation in decision-making, public and social services, transparent governance, and political strategies and perspectives. The chapter presents sustainability of smart governance through a paradigm of sustainability as an effectual model based on sustainability, wellbeing, productivity, and resilience. Finally, the chapter addresses the success criteria of sustainable smart cities regarding different aspects, such open data, agility to new technologies, cross-sectoral harmonization, and careful policy, strategy, and program alignment.