Phytotechnologies used for cleaning up urban and suburban polluted soils (i.e., brownfields) have shown some weakness in the excessive extent of the timeframe required for them to be effectively operating. This bottleneck is due to technical constraints, mainly related to both the nature of the pollutant itself (e.g., low bio-availability, high recalcitrance, etc.) and the plant (e.g., low pollution tolerance, low pollutant uptake rates, etc.). Despite the great efforts made in the last few decades to overcome these limitations, the technology is in many cases barely competitive compared with conventional remediation techniques. Here, we propose a new outlook on phytoremediation, where the main goal of decontaminating should be re-evaluated, considering additional ecosystem services (ESs) related to the establishment of a new vegetation cover on the site. The aim of this review is to raise awareness and stress the knowledge gap on the importance of ES associated with this technique, which can make phytoremediation a valuable tool to boost an actual green transition process in planning urban green spaces, thereby offering improved resilience to global climate change and a higher quality of life in cities. This review highlights that the reclamation of urban brownfields through phytoremediation may provide several regulating (i.e., urban hydrology, heat mitigation, noise reduction, biodiversity, and CO2 sequestration), provisional (i.e., bioenergy and added-value chemicals), and cultural (i.e., aesthetic, social cohesion, and health) ESs. Although future research should specifically be addressed to better support these findings, acknowledging ES is crucial for an exhaustive evaluation of phytoremediation as a sustainable and resilient technology.