Nature-based solutions (NbS) provide direct benefits to people who live in areas where these approaches are present. The degree of direct benefits (thermal comfort, reduced flood risk, and mental health) varies across temporal and spatial scales, and it can be modelled and quantified. Less clear are the indirect benefits related to opportunities to learn about the environment and its influence on personal behaviour and action. The present study, based on survey data from 1955 participants across 17 cities worldwide, addressed whether participation in NbS through two types of interactions (a passive learning experience about NbS and a more active experience based on Citizen Science) stimulates motivation and willingness to be more environmentally sustainable. Over 75% of participants improved their understanding of environmental sustainability and were highly motivated and more confident in their ability to improve sustainability in their local environment/nature. Similar percentage improvements arose from both types of activity across all cities. Those NbS that had elements of both blue and green infrastructure rated higher than those that had predominantly green NbS. Interestingly, a large percentage of the participants did not live near the NbS that were the focus of these activities. This indicated that expected spatial limitations between benefit and recipient may be overcome when dedicated programmes involve people in learning or monitoring NbS. Therefore, opportunities have arisen to expand inclusion from the immediately local to the larger community through participation and Citizen Science, with potential benefits to social cohesion and urban sustainability.