The purpose of this chapter is to explore mechanisms and potentials for measuring ambient urbanities. This work advances the ambient metrics concept as a way of shedding light on the evolving nature of measures, standards, and indices required by more dynamic, adaptive, and aware environments, characteristic of smart and responsive cities. In the form of ambient metrics, measures are sought that support more informed city experiences, increased engagement and participation, and improved quality of urban life. The research literature for smart city metrics, standards, and indices is explored in this chapter enabling identification of issues, controversies, and problems. Using an exploratory case study approach, solutions and recommendations are advanced. This chapter makes a contribution to the research literature for smart city metrics, standards, and indices; the evolving of urban theory for 21st century cities; and urban theory in formulating a conceptual framework for rethinking measures for smarter urbanities.