The use of nature-based solutions (NbS) in urban regeneration processes has been demonstrated as a multifunctional solution to increase the resilience of the built environment, contributing to improved environmental quality and health and wellbeing, and providing empowerment to communities facing natural hazards. However, when it comes to the assessment of psychological wellbeing and social benefits, existing evidence is still limited. To contribute to the knowledge of NbS’ psychosocial benefits, it is necessary to develop and test assessment tools to contribute to a common NbS monitoring framework. In this paper, we describe the development of a psychosocial benefit assessment tool for nature-based interventions in the urban regeneration processes. This tool has been developed within the framework of the H2020 CLEVER-Cities project through a participatory and co-design process, considering advanced sustainability paradigms, such as Regenerative Sustainability and Sensory Sustainability Science. This tool is structured around two dimensions, (1) perceived health and wellbeing and (2) social benefits, which refer to 13 attributes, assessed through 24 items. The Delphi method was used to validate the assessment tool, in which a multidisciplinary panel of experts participated. The results indicate that it has good face and content validity, concluding with the potential applicability of this tool in different contexts.