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Green infrastructures deliver countless functions for counteracting climate change, air pollution, floods, and heat islands, contributing at the same time to water and carbon recycling as well as to renewable energies and feedstock provisioning. Properly addressing such environmental problems would require huge investments that could be decreased thanks to the further implementation of urban forests. Local administrations are designing participative projects to improve territories and their living conditions. The i-Tree Canopy modelling tool and the life cycle assessment method are jointly applied to evaluate the potential benefits of increasing tree coverage within the boundaries of the Metropolitan City of Naples, Southern Italy. Results highlighted that tree coverage could increase by about 2.4 million trees, thus generating 51% more benefits in pollutants removal, carbon sequestration and stormwater management. The benefits are also explored and confirmed by means of the life cycle assessment method. The potential tree cover is expected to provide a total annual economic benefit of USD 55 million, purchasing power parity value adjusted, representing USD 18 per citizen and USD 99,117 per square kilometre of implemented urban forest. These results can support a potential replication elsewhere and provide a reference for the sustainable improvement of cities by expanding urban green areas.