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The analysis of urban sustainability is key to urban planning, and its usefulness extends to smart cities. Analyses of urban quality typically focus on applying methodologies that evaluate quality objectives at environmental, urban, and building levels. Research has shown that a system of indicators can be useful for developing qualitative and quantitative descriptors of urban environments. The first step in this study was to formulate a methodology to measure the quality of urban life based on investigative checklists and objective and subjective indicators, aggregated to develop an index to evaluate a city’s level of smart urban quality. The second step was to apply this methodology to evaluate the city of Cagliari (Italy) at the neighbourhood scale, which is considered by literature the most suitable as a self-sufficient spatial unit for showing redevelopment results. In addition to sharing its research findings, this study aims to verify whether the methodology can be applied to similar urban contexts. The main outcomes of this research pertain to opportunities to numerically measure both objective and subjective aspects that affect urban quality. In this way, the most critical areas to be requalified have been highlighted in order to prepare policies congruent with the local context.