This article examines the ways in which ‘nature-based solutions’ (NBS) to urban environmental problems are contributing to a re-imagining of the forms and roles of vegetal life in cities. Specifically, we examine the versions of nature that are being produced within a subset of nature-based solutions described as ‘smart’ – that is, those involving the enrolment of non-human lifeforms into digital infrastructures comprising sensors, data flows and automated support systems. Whilst NBS are often celebrated for opening up cities to lively ecological processes – thereby contributing to more convivial, ‘more-than-human’ forms of urbanism – their smart incarnations are becoming a playground for entrepreneurial and financial actors seeking new ways to enclose, commodify and derive profit from non-human life in cities. To explicate this argument, we examine the case of a proprietary ‘nature-based solution’ to urban air pollution developed and sold to local authorities and corporate actors by a European cleantech start-up, predicated on optimising the air-filtering capacities of moss. Our analysis proceeds in three stages. First, we draw on scholarship on the bioeconomy to show how the commodification of moss in this case is predicated on discursive arguments which depict moss as at once inherently productive and regenerative, but also fragile and scarce in urban environments. Secondly, we show how this smart NBS is rendered investable through the enrolment of moss into a carefully designed digital apparatus, which purports to stabilise and optimise its air purifying work, thereby making its contributions to urban air quality continuous, consistent and calculable. Finally, building on an assessment of the entanglement of this example with specific urban geographies and modes of urban governance, we critically reflect on the role that smart NBS in general might yet play in either reinforcing or disrupting prevailing dynamics of privatisation, enclosure and green gentrification in cities.