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Urban sprawl has several negative impacts on the environment, the economy, and human health. The main objective of this work was to formulate and validate a sprawl/compactness index for Sicilian municipalities and evaluate its association with health outcomes. An ecological study was conducted with 110 municipalities in Sicily, Italy. Principal component analysis was adopted to create the sprawl/compactness Sicilian index, and linear regression analysis was used to evaluate the association between the sprawl index and health outcomes. More variance of the new sprawl index was explained by the working factor, followed by density, surface extension, and land use mix. When validating the index, we found that public transportation had an inverse relation with sprawl increase ( p < 0.001), and private transportation was directly related to the increase in sprawl ( p < 0.001). After controlling for the Sicilian socio-economic deprivation index and overall mortality, cardiovascular mortality was the only outcome directly associated with the increase in the sprawl index (odds ratio = 0.0068, p < 0.001). Urban sprawl has to be monitored in Sicily over time to understand the evolution of the urbanization phenomenon and its relationship with health outcomes such as cardiovascular mortality. The use of the sprawl index should help policymakers define the necessary strategic aspects and actions to improve human health and quality of life in cities through a multi-sectorial approach.